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Abstract In the past century, ferroelectrics are well known in electroceramics and microelectronics for their unique ferroelectric, piezoelectric, pyroelectric, and photovoltaic effects. Nowadays, the advances in understanding and tuning of these properties have greatly promoted a broader application potential especially in energy and environmental fields, by harvesting solar, mechanical, and heat energies. For example, high piezoelectricity and high pyroelectricity can be designed by defect or microstructure engineering for piezo‐ and pyro‐catalyst, respectively. Moreover, highly piezoelectric and broadband (UV–Vis–NIR) light‐responsive ferroelectrics can be designed via defect engineering, giving rise to a new concept of photoferroelectrics for efficient photocatalysis, piezocatalysis, pyrocatalysis, and related cocatalysis. This article first summarizes the recent developments in ferroelectrics in terms of piezoelectricity, pyroelectricity, and photovoltaic effects based on defect and microstructure engineering. Then, the potential applications in energy generation (i.e., photovoltaic effect, H2 generation, and self‐powered multisource energy harvesting and signal sensing) and environmental protection (i.e., photo‐piezo‐pyro‐ cocatalytic dye degradation and CO2 reduction) are reviewed. Finally, the outlook and challenges are discussed. This article not only covers an overview of the state‐of‐art advances of ferroelectrics, but also prospects their applications in coping with energy crisis and environmental pollution.

(Na0.5Bi0.5)TiO3 (NBT)-based materials have been widely studied for their large electric-field-induced strains. However, a high coercive field (Ec) has long hindered the applications of NBT-based materials. Here, we propose a simple method to significantly reduce the Ec of rhombohedral NBT-based crystals through domain engineering. By applying an alternating current (AC) electric field along the [001] direction, the Ec of Mn-doped (Na0.485K0.015Bi0.5)TiO3 single crystal can be reduced from 70 to 20 kV/cm after about 25 cycles without sacrificing the ferroelectric polarization. Meanwhile, the piezoelectric coefficient d33 and the optical transparency of the crystals are also enhanced compared with those after direct-current electric field poling. The domain structure characterization shows that the AC cycles can form a laminar domain configuration, in which the 109° domain walls are parallel to (001) planes. It is demonstrated that in the laminar domain configuration, almost only 71° polarization switching occurs when the external electric field is reversed. The required energy for polarization reversal is significantly lower than that of the "4R" domain configuration; thus, the Ec is reduced greatly. The low Ec is maintained after depolarization at 250 °C, evidencing good thermal stability of the laminar domain configuration. Furthermore, this method is also applicable to other rhombohedral single crystals and may be applied to [001]-textured polycrystalline ceramics in the future; thus, it may indeed benefit the practical applications of NBT-based piezoelectric devices. [ABSTRACT FROM AUTHOR]

Lead‐free piezoelectric ceramics with excellent piezoelectric performance and temperature stability are vital to "stack up" against PZT in various applications. Thus, xBiFeO3‐(1‐x)BaTiO3(BF‐BT)‐based ceramics with high Curie temperatures have drawn increasing attention. However, BF‐BT based ceramics often show large leakage current due to the valence fluctuation of Fe ion. In this work, it is found that Bi(Ni2/3Nb1/3)O3 (BNN) can suppress the valence fluctuation of Fe ions effectively. The effects of BNN on the crystal structure, morphology, and electrical properties of 0.69BF‐0.31BT ceramics are investigated. For composition near morphotropic phase boundary of rhombohedral and tetragonal phases, the Curie temperature (Tc) is as high as 453°C, and the piezoelectric constant (d33), planar electromechanical coupling factor kp, and electric‐field‐induced strain ΔS can reach up to 191 pC/N, 31% and 0.236% (peak to peak), respectively. Moreover, these ceramics show excellent thermal stability. The d33 of 100 pC/N is still maintained at about 360°C and an ultrahigh strain (ΔS = 0.684%, peak to peak strain) is obtained at 190°C. Our work illustrates that the BF‐BT based ceramics can serve as potential candidates for sensor and actuator applications over a broad temperature range. [ABSTRACT FROM AUTHOR]

Lead-free piezoelectric actuators emerge as promising substitutes for their lead-containing counterparts to address environmental concerns. However, they often confront a trade-off between low driving electric fields and high electro-strain. Herein, a novel strategy to boost electro-strain under low electric fields is proposed by doping high-electronegativity B-site atoms into perovskite potassium sodium niobate-based ceramics. Our findings reveal that high-electronegativity B-site atoms elevate the covalency of B-O bonding, softening the short-range repulsion and introducing local multiphase coexistence. This leads to more nanoscale domain structures and lower coercive field, thereby enabling large strains to be produced at lower electric fields. Notably, a substantial 0.2 % bipolar electro-strain and 0.1 % unipolar electro-strain under 10 kV cm-1 is achieved in Sr, Sb co-doped potassium sodium niobate ceramics, with a broad working frequency and temperature range, as well as excellent fatigue resistance. This study unveils innovative insights into designing lead-free piezoelectric ceramics with remarkable electro-strain performance and low driving electric field, promising a significant advancement in lead-free piezoelectric materials science and piezoelectric actuators. [Display omitted] [ABSTRACT FROM AUTHOR]

The development of ultrathin (≤5 nm) hafnia‐based ferroelectric (FE) films is essential for achieving low operating voltages, facilitating their integration into advanced process nodes for low‐power and non‐volatile memory applications. However, challenges in ultrathin FE films arise from the depolarization field and interface‐related issues, leading to an antiferroelectric‐like (AFE‐like) polarization switching behavior and more significant wake‐up effects, causing operational inconvenience and reliability concerns. Here, interface‐modulated ferroelectricity is reported in 4 nm Hf0.5Zr0.5O2 (HZO) thin films, demonstrating excellent properties with low operating voltage, enhanced switching speed, and high reliability. Electrical and structural characterizations reveal that adjusting interface asymmetry may introduce a substantial built‐in field (Ebi) and an AFE‐like switching behavior can exhibit a robust FE‐like characteristic. This AFE‐to‐FE‐like transition is driven by switching kinetics rather than commonly proposed phase transitions. Furthermore, a comprehensive model is developed to elucidate the intricate physics of the modulation mechanism by asymmetric interfaces, emphasizing the critical roles of depolarizing effects and Ebi on ferroelectricity. This work underscores the importance of interfaces in engineering ferroelectricity for advanced electronic applications. [ABSTRACT FROM AUTHOR]

The comprehensive understanding of (Na 0.5 Bi 0.5 )TiO 3 -BaTiO 3 (NBT-BT) lattice structure is highly desired to develop lead-free ferroelectric materials. However, most of the previous studies focused on the improvement of piezoelectric properties at room temperature, and many structural puzzles are left unclear. In this work, the lattice structure of a ferroelastic phase and the ferroelectric-ferroelastic transitions in both rhombohedral NBT and tetragonal NBT-8%BT single crystals are investigated in detail. Our results illustrate the complex process of the ferroelectric-ferroelastic transition of NBT. The variation of Ti-O modes and oxygen octahedra modes clearly indicates the gradual change of lattice symmetry from R 3 c to P 4 bm during a wide temperature range between 170 and 350 °C. A ferroelectric-ferroelastic transition is also confirmed in tetragonal NBT-8BT for the first time, and the lattice symmetry of P 4 bm is found to be maintained during the ferroelastic stage. This work reveals the lattice evolutions of the ferroelectric-ferroelastic transition of NBT-BT crystals and provides new insights for understanding the ferroelasticity and the evolution of phonon modes in a lead-free relaxor.