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The benefits of the multiphase convergence strategy to design ferroelectric ceramics for piezoelectric energy harvesting applications over a broad temperature range.

The energy storage performances in ceramic/polymer nanocomposites are mainly linked to the dielectric permittivity and the aspect ratio of the nanofiller, though, the morphological effect (aspect ratio) is greater than the permittivity one.

International audience; Ba0.85Ca0.15Zr0.10Ti0.90O3 (BCZT) relaxor ferroelectric ceramics exhibit enhanced energy storage and electrocaloric performances due to their excellent dielectric and ferroelectric properties. In this study, the temperature-dependence of the structural and dielectric properties, as well as the field and temperature-dependence of the energy storage and the electrocaloric properties in BCZT ceramics elaborated at low-temperature hydrothermal processing are investigated. X-ray diffraction and Raman spectroscopy results confirmed the ferroelectric–paraelectric phase transition in the BCZT ceramic. At room temperature and 1 kHz, the dielectric constant and dielectric loss reached 5000 and 0.029, respectively. The BCZT ceramic showed a large recovered energy density (Wrec) of 414.1 mJ cm−3 at 380 K, with an energy efficiency of 78.6%, and high thermal-stability of Wrec of 3.9% in the temperature range of 340–400 K. The electrocaloric effect in BCZT was explored via an indirect approach following the Maxwell relation at 60 kV cm−1. The significant electrocaloric temperature change of 1.479 K at 367 K, a broad temperature span of 87 K, an enhanced refrigerant capacity of 140.33 J kg−1, and a high coefficient of performance of 6.12 obtained at 60 kV cm−1 make BCZT ceramics potentially useful coolant materials in the development of future eco-friendly solid-state refrigeration technology.

Lead-free BaTi0.89Sn0.11O3 (BTSn) ceramic was elaborated via a solid-state reaction method and its dielectric, ferroelectric, energy storage, electromechanical as well as electrocaloric properties were investigated at 25 kV/cm. Pure perovskite structure was confirmed by X-ray diffraction analysis. The maximum of the dielectric constant was found to be 17390 at 41 °C. The enhanced total energy density, the recovered energy density, and the energy storage efficiency of 92.7 mJ/cm3, 84.4 mJ/cm3, and 91.04 %, respectively, were observed at 60 °C. In contrast, the highest energy storage efficiency of 95.87 % was obtained at 100 °C. At room temperature, the electromechanical strain and the large-signal piezoelectric coefficient reached a maximum of 0.07 % and 280 pm/V. The large electrocaloric effect of 0.71 K and the electrocaloric responsivity of 0.28 × 10-6 K mm/kV at 49 °C under 25 kV/cm were indirectly determined via Maxwell approach and the measured ferroelectric polarization P(T,E). The electrocaloric response was also modelled by exploiting the Landau-Ginzburg-Devonshire (LGD) phenomenological theory. The modelling result of 0.61 K at 50 °C under 25 kV/cm supports the experimental findings. We conclude that BTSn lead-free ceramic is a promising candidate for potential applications in high-efficiency energy storage devices and solid-state refrigeration technology.

The lead-free Ba0.85Ca0.15Zr0.10Ti0.90O3 (BCZT) relaxor ferroelectric ceramic has aroused much attention due to its enhanced piezoelectric, energy storage and electrocaloric properties. In this study, the BCZT ceramic was elaborated by the solid-state reaction route, and the temperature-dependence of the structural, electrical, piezoelectric, energy storage and electrocaloric properties was investigated. X-ray diffraction analysis revealed a pure perovskite phase, and the temperature-dependence of Raman spectroscopy, dielectric and ferroelectric measurements revealed the phase transitions in the BCZT ceramic. At room temperature, the strain and the large-signal piezoelectric coefficient reached a maximum of 0.062% and 234 pm V−1, respectively. Furthermore, enhanced recovered energy density (Wrec = 62 mJ cm−3) and high-energy storage efficiency (η) of 72.9% at 130 °C were found. The BCZT ceramic demonstrated excellent thermal stability of the energy storage variation (ESV), less than ±5.5% in the temperature range of 30–100 °C compared to other lead-free ceramics. The electrocaloric response in the BCZT ceramic was explored via the indirect approach by using the Maxwell relation. Significant electrocaloric temperature change (ΔT) of 0.57 K over a broad temperature span (Tspan = 70 °C) and enhanced coefficient of performance (COP = 11) were obtained under 25 kV cm−1. The obtained results make the BCZT ceramic a suitable eco-friendly material for energy storage and solid-state electrocaloric cooling devices.

International audience; Lead-free Ba0.85Ca0.15Zr0.10Ti0.90O3 (BCZT) ceramics have demonstrated excellent dielectric, ferroelectric, and piezoelectric properties in comparison to lead-based materials. The synthesis of pure and crystalline BCZT nanopowders at low temperatures of 25, 80, and 160 °C was reported previously by using a sol–gel method followed by a hydrothermal route. In this study, the structural, dielectric, and ferroelectric properties of sintered BCZT ceramics at 1250 °C/10 h were investigated. XRD measurements revealed the presence of a single perovskite phase at room temperature with the coexistence of the orthorhombic and tetragonal symmetries. The increase of grain size and the ceramic density in BCZT ceramics result in an enhancement of the dielectric and ferroelectric properties of BCZT ceramics. More interestingly, the synthesis temperature of BCZT powders with high dielectric and ferroelectric properties could be decreased to a low temperature of 160 °C, which is about 1200 °C lower when compared with solid-state reaction and 840 °C lower when compared with sol–gel methods. The BCZT ceramics elaborated at 160 °C revealed excellent electrical properties (dielectric constant, dielectric loss, remnant polarization, and maximal polarization of 12,085, 0.017, 8.59 µC/cm2, and 27.21 µC/cm2, respectively) and enhanced energy performances (recovered energy density and energy efficiency of 367.2 mJ/cm3 and 67.2%, respectively). Hence, the use of low-temperature hydrothermal processing can be encouraging for the synthesis of lead-free ceramics with high dielectric and ferroelectric properties.

International audience; The effects of 2% Zr introduction in Ba0.8Ca0.2TiO3 (BCT) system on its electrical and electrocaloric properties was investigated. BCT and Ba0.8Ca0.2Zr0.02Ti0.98O3 (BCZT) ceramics synthesized by solid-state processing were crystallized in a pure perovskite phase with a group space P4mm. After Zr insertion, the enhanced dielectric constant was obtained around the Curie temperature (Tc) in BCZT ceramic (εr = 6330 at Tc = 388 K) compared to BCT ceramic (εr = 5080 at Tc = 388.6 K). Moreover, the large-signal piezoelectric coefficient (d∗33) was improved from 270 to 310 pm/V in BCT and BCZT ceramics, respectively, under a moderate electric field of 25 kV/cm. The electrocaloric effect was determined via indirect and direct methods. In the indirect approach, the electrocaloric temperature change (ΔT) was calculated via Maxwell relation, and the measured ferroelectric polarization P (E, T) extracted from the P–E curves recorded at 24 kV/cm. The maximum values of ΔT = 0.68 K and the electrocaloric responsivity ζ = 0.283 K mm/kV obtained at 385 K in BCZT ceramic were found to be higher than those observed in BCT ceramic (ΔT = 0.37 K and ζ = 0.154 K mm/kV at 387 K). In the direct approach, ΔT was measured utilizing a modified high-resolution calorimeter at 14 kV/cm. As the direct method is more sensitive to the latent heat, it provided larger values for smaller applied field, i.e., ΔT = 0.474 and 0.668 K for BCT and BCZT ceramics, respectively. A significant ζ of 0.477 K mm/kV was obtained in BCZT at 385 K and 14 kV/cm that matches the values found in lead-based materials. These results suggest that BCZT lead-free ceramics could have an excellent potential to be used in solid-state refrigeration applications.

International audience; Lead-free Ba0.85Ca0.15Zr0.10Ti0.90O3 (BCZT) ceramic exhibits excellent dielectric, ferroelectric and piezoelectric properties at the morphotropic phase boundary (MPB). Previously, we demonstrated that the use of the anionic surfactant sodium dodecyl sulfate (SDS, NaC12H25SO4) could enhance the dielectric properties of BCZT ceramic using surfactant-assisted solvothermal processing [1]. In the present study, structural, dielectric, ferroelectric properties, as well as electrocaloric effect and energy storage performances of this BCZT ceramic were thoroughly investigated. X-ray diffraction (XRD) measurements revealed the presence of single perovskite phase at room temperature with the coexistence of orthorhombic and tetragonal symmetries. In-situ Raman spectroscopy results confirmed the existence of all phase transitions from rhombohedral through orthorhombic and tetragonal to cubic symmetries when the temperature varies as reported in undoped-BaTiO3. Evolution of energy storage performances with temperature have been investigated. BCZT ceramic exhibits a high energy storage efficiency of ~ 80% at 120 °C. In addition, the electrocaloric responsivity was found to be 0.164 × 10−6 K·m/V at 363 K.

International audience; The site-doping strategy of barium titanate (BaTiO3) is a promising way to develop new lead-free materials for energy with enhanced dielectric and piezoelectric properties. A novel strategy to elaborated pure and crystalline Ba.85Ca.15Zr.1Ti.9O3 (BCZT) ferroelectric powders at low temperature is proposed. It is based on sol-gel method followed by a hydrothermal reaction. The effects of preparation temperature on structure, crystallinity, purity, morphology and particles size distribution of BCZT powders were studied. It was clearly shown that pure and crystalline BCZT could be obtained over 80 °C. Furthermore, the BCZT particles exhibit a spherical shape whose mean size increases from 145 nm at 40 °C to 160 nm at 80 °C. The present study may provide a new strategy to design lead-free ferroelectric materials with enhanced structure and microstructure properties at very low temperature.

Lead-free Ba0.85Ca0.15Ti0.9Zr0.1O3 (BCZT) ceramics had attracted much attention for the fabrication of microelectronic devices by virtue of their excellent dielectric, ferroelectric and piezoelectric properties. To understand the effects of both mean grain size and grain size distribution on the dielectric properties of lead-free Ba0.85Ca0.15Ti0.9Zr0.1O3 (BCZT) ferroelectric relaxors, an original method was proposed. It is based on the surfactant-assisted solvothermal processing coupled with low-temperature conventional sintering at 1250 {\deg}C. In this way, three highly dense BCZT with different mean grain size and dissimilar grain size distribution were designed. A significant increase of dielectric properties was obtained by a control of grain size and densification process. The dielectric constants measured were ranged from 5370 to 9646 and the dielectric loss was enhanced by 70%. Surprisingly, it was evidenced that there is unequivocal link between mean grain size with dielectric properties. Indeed, it was found that the presence of high density of refined grains leads to an improvement of dielectric properties due to an enhancement of densification. This work may provide a new strategy to design ferroelectric materials with enhanced properties., Comment: Superlattices and Microstructures 2018

Design of a low-cost, eco-friendly, self-poled and flexible piezoelectric nanogenerator based on lead-free H2(Zr0.1Ti0.9)3O7 piezo-nanowires and polylactic acid biodegradable piezopolymer.

Mechanical energy harvesting using piezoelectric nanogenerators (PNGs) offers an attractive solution for driving low-power portable devices and self-powered electronic systems. Here, we designed an eco-friendly and flexible piezocomposite nanogenerator (c-PNG) based on H

International audience; Piezoelectric nanogenerators are attracting substantial attention due to the environmental constraints and ecological considerations of energy harvesting. However, the Achilles' heel of the majority of these nanogenerators is the presence of toxic compounds or the requirement of a poling process to promote higher piezoelectric effect. Here, a self-poled and bio-flexible piezoelectric nanogenerator (BF-PNG) is designed, based on lead-free biocompatible Ba0.85Ca0.15Zr0.10Ti0.90O3 nanoparticles that are functionalized with polydopamine and embedded in the polylactic acid biodegradable polymer. The BF-PNG can generate open-circuit voltage and short-circuit current of 14.4 V and 0.55 µA, respectively, under gentle finger tapping. Furthermore, it demonstrates an outstanding high mechanical robustness, stable and durable output even after one year. It achieves a maximum power density of about 7.54 mW/cm3 at a low resistive load of 3.5 MΩ. The feasibility of the BF-PNG by trigging commercial electronics such as charging capacitors and lighting a LED is verified, and the BF-PNG can drive a 1 µF capacitor to store the energy of 3.92 µJ within 115 s under gentle finger tapping. This research demonstrates that a lead-free piezoceramic in combination with a biodegradable piezopolymer can lead to a design of bio-flexible piezoelectric nanogenerators with outstanding performances and in particular useful in self-powered medical devices.