Single phase PbHfO 3 antiferroelectric ceramics were prepared via rolling process. It is revealed that the rolling process can reduce the grain size and increase the bulk density, which lead to the enhanced breakdown strength up to 268 kV/cm versus 219 kV/cm of samples using the conventional solid-state method. As a result, high recoverable energy density of 7.6 J/cm 3 with an efficiency of 80.8 % was achieved. Meanwhile, a large current density of 1381 A/cm 2 and an ultrahigh peak power density up to 170 MW/cm 3 were observed under 250 kV/cm. In addition, unique electrical polarization response characteristics at different electric fields and temperature-induced structural phase transitions were also investigated. The energy storage performance and charge-discharge properties of PbHfO 3 were first studied in this communication and all the results indicate that PbHfO 3 ceramic is a promising candidate for pulse power applications.
Antiferroelectric materials exhibit fantastic application potential in multifunctional devices due to their special structure and polarization/strain-electric field responses. However, it has long been challenging to realize multifunctionality in PbHfO 3 , one of the prototypical antiferroelectrics, due to its poor sinterability and structural complexity. To address these issues, we report an effective strategy to obtain fine and dense PbHfO 3 ceramics by the solid-state reaction method involving a liquid phase sintering mechanism. The crystal structure, microstructure, phase transitions, energy storage, and strain performance are systematically investigated. A high recoverable energy density W reco (7.29 J/cm 3 ) and a large strain (0.51%) are achieved with a temperature-stable (25 ∼ 175 °C) feature. By combination of synchrotron and laboratorial X-ray diffraction, Raman spectroscopy, dielectric and impedance spectroscopy, and density-functional-theory calculations, the high and temperature-stable energy-storage and strain properties are determined to arise from the stable antiferroelectric nature of PbHfO 3 with a large polarization in a broad temperature range and its transformation to a ferroelectric phase with R 3 c symmetry under electric field. Furthermore, the ceramics present a negative temperature coefficient of resistance in a higher temperature range of 400 ∼ 600 °C. These performances grant PbHfO 3 antiferroelectric ceramics a huge potential for applications in high-density energy storage capacitors, large-displacement actuators, and temperature sensors and compensators over a broad temperature range.
Antiferroelectric (AFE) materials have gained significant attention due to their potential multifunctionality. However, prototypical AFE materials, such as PbHfO3, suffer from poor sinterability, complex structures, and a high critical electric field, making it difficult for them to achieve expected performances. Here we adopt a synergistic design strategy, namely by inducing ferroelectrically active ions into the PbHfO3 structural matrix to soften the AFE order and induce a large maximum polarization, to enable the development of novel PbHfO3-based AFE materials of high performance suitable for applications under low electric fields. To implement this strategy, a novel solid solution of (1 − x)PbHfO3–xPb(Zn1/2W1/2)O3 is designed and prepared by the solid-state reaction method. Its crystal structure, microstructures, energy storage and strain performances, and phase transition behaviors are systematically investigated from both experimental and theoretical aspects. The resulting material exhibits a high recoverable energy storage density of 5.03 J cm−3 and a large strain of 0.60% under a relatively low electric field of 200 kV cm−1, which proves the effectiveness of our synergistic strategy. Phenomenological modeling investigation associates these performances with the sharp jump in induced polarization and strain, which is consistent with the experimental results. This work not only results in a novel AFE candidate material for high energy storage and strain applications but also, more importantly, opens up a new way to design high-performance AFE materials with multifunctionality via softening the AFE order.
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