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The integration of metal oxides onto two-dimensional layered siloxene has proven to be an effective strategy for expanding potential applications across diverse fields. Herein, we present the synthesis and detailed characterization of zinc oxide (ZnO) nanorods deposited on siloxene nanosheets using the wet chemical precipitation method without the need of alkali. The presence of ZnO nanorods was confirmed through electron microscopy analyses. X-ray diffraction analysis further verified the presence of characteristic peaks of ZnO in the hexagonal wurtzite crystal structure. Dielectric measurements demonstrated the moderated stability of interfacial polarization in siloxene nanosheets doped with zinc oxide (SX-ZnO) over a broad frequency spectrum, coupled with minimal electrical loss values under 0.4 within the 100 Hz to 1 MHz frequency range. In addition, the ferroelectric study of SiNSs-ZnO composites revealed a slim hysteresis loop with maximum polarization and remnant polarization values that varied with reaction times. The SX-ZnO sample prepared for 5 h exhibited the best stored energy properties, featuring a moderate stored energy density (Ws = 771.94 mJ cm-3) and a high energy efficiency of 83.38%. This investigation underscores that the modification of siloxene layers through the deposition of nanostructured transition metal oxide materials leads to stabilized interfacial polarization and enhanced efficient energy storage.
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In the most recent electronic and electric sectors, ceramic-polymer nanocomposites with high dielectric permittivity and energy density are gaining popularity. However, the main obstacle to improving the energy density in flexible nanocomposites, besides the size and morphology of the ceramic filler, is the low interfacial compatibility between the ceramic and the polymer. This paper presents an alternative solution to improve the dielectric permittivity and energy storage properties for electronic applications. Here, the poly(vinylidene fluoride-hexafluoropropylene) (PVDF-HFP) matrix is filled with surface-modified BaTi0.89Sn0.11O3/polydopamine nanoparticles (BTS11) nanoparticles, which is known for exhibiting multiphase transitions and reaching a maximum dielectric permittivity at room temperature. BTS11 nanoparticles were synthesized by a sol-gel/hydrothermal method at 180 °C and then functionalized by polydopamine (PDA). As a result, the nanocomposites exhibit dielectric permittivity (εr) of 46 and a low loss tangent (tan δ) of 0.017 at 1 kHz at a relatively low weight fraction of 20 wt% of BTS11@PDA. This is approximately 5 times higher than the pure PVDF-HFP polymer and advantageous for energy storage density in nanocomposites. The recovered energy storage for our composites reaches 134 mJ cm-3 at an electric field of 450 kV cm-1 with a high efficiency of 73%. Incorporating PDA-modified BTS11 particles into the PVDF-HFP matrix demonstrates highly piezo-active regions associated with BTS11 particles, significantly enhancing functional properties in the polymer nanocomposites.
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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 H2(Zr0.1Ti0.9)3O7 nanowires (HZTO-nw) and Ba0.85Ca0.15Zr0.10Ti0.90O3 multipods (BCZT-mp) as fillers and polylactic acid (PLA) as a biodegradable polymer matrix. The effects of the applied stress amplitude, frequency and pressing duration on the electric outputs in the piezocomposite nanogenerator (c-PNG) device were investigated by simultaneous recording of the mechanical input and the electrical outputs. The fabricated c-PNG shows a maximum output voltage, current and volumetric power density of 11.5 V, 0.6 µA and 9.2 mW cm-3, respectively, under cyclic finger imparting. A high-pressure sensitivity of 0.86 V kPa-1 (equivalent to 3.6 V N-1) and fast response time of 45 ms were obtained in the dynamic pressure sensing. Besides this, the c-PNG demonstrates high-stability and durability of the electrical outputs for around three months, and can drive commercial electronics (charging capacitor, glowing light-emitting diodes and powering a calculator). Multi-physics simulations indicate that the presence of BCZT-mp is crucial in enhancing the piezoelectric response of the c-PNG. Accordingly, this work reveals that combining 1D and 3D fillers in a polymer composite-based PNG could be beneficial in improving the mechanical energy harvesting performances in flexible piezoelectric nanogenerators for application in electronic skin and wearable devices.
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Ferroelectric property that induces electrocaloric effect was investigated in Ba(GexTi1-x)O3 ceramics, known as BTGx. X-ray diffraction analysis shows pure perovskite phases in tetragonal symmetry compatible with the P4mm (No. 99) space group. Dielectric permittivity exhibits first-order ferroelectric-paraelectric phase transition, confirmed by specific heat measurements, similar to that observed in BaTiO3 (BTO) crystal. Curie temperature varies weakly as a function of Ge-content. Using the direct and indirect method, we confirmed that the adiabatic temperature change ΔT reached its higher value of 0.9 K under 8 kV/cm for the composition BTG6, corresponding to an electrocaloric responsivity ΔT/ΔE of 1.13 × 10-6 K.m/V. Such electrocaloric responsivity significantly exceeds those obtained so far in other barium titanate-based lead-free electrocaloric ceramic materials. Energy storage investigations show promising results: stored energy density of ~17 mJ/cm3 and an energy efficiency of ~88% in the composition BTG5. These results classify the studied materials as candidates for cooling devices and energy storage applications.
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The design of lead-free ceramics for piezoelectric energy harvesting applications has become a hot topic. Among these materials, Ba0.85Ca0.15Zr0.10Ti0.90O3 (BCZT) and BaTi0.89Sn0.11O3 (BTSn) are considered as potential candidates due to their enhanced piezoelectric properties. Here, the structural, electrical, piezoelectric and piezoelectric energy harvesting properties of the (1 - x)Ba0.85Ca0.15Zr0.10Ti0.90O3-xBaTi0.89Sn0.11O3 (xBTSn, x = 0.2, 0.4 and 0.6) system are investigated. A systematic study of the structural properties of the xBTSn samples was carried out using X-ray diffraction, Raman spectroscopy, and dielectric measurements. The addition of BTSn allows a successive phase transition, which broadens the application temperature range. The enhanced piezoelectric energy harvesting properties were found in the 0.2BTSn ceramic, where the large-signal and small-signal piezoelectric coefficients, piezoelectric voltage and the piezoelectric figure of merit reached 245 pm V-1, 228 pC N-1, 16.2 mV m N-1 and 3.7 pm2 N-1, respectively. Consequently, the combination of BCZT and BTSn could provide suitable lead-free materials with enhanced piezoelectric energy harvesting performances.
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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 (W rec = 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 (T span = 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.
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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 (W rec) of 414.1 mJ cm-3 at 380 K, with an energy efficiency of 78.6%, and high thermal-stability of W rec 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.