Multiscale Structural Engineering Boosts Piezoelectricity in Na0.5Bi2.5Nb2O9-Based High-Temperature Piezoceramics.

High-temperature piezoelectric materials, which enable the accurate and reliable sensing of physical parameters to guarantee the functional operation of various systems under harsh conditions, are highly demanded. To this end, both large piezoelectricity and high Curie temperature are pivotal figures of merit (FOMs) for high-temperature piezoceramics. Unfortunately, despite intensive pursuits, it remains a formidable challenge to unravel the inverse correlation between these FOMs. Herein, a conceptual material paradigm of multiscale structural engineering was proposed to address this dilemma. The synergistic effects of phase structure reminiscent of a polymorphic phase boundary and refined domain morphology simultaneously contribute to a large piezoelectric coefficient d33 of 30.3 pC/N and a high Curie temperature TC of 740 °C in (LiCeNd) codoped Na0.5Bi2.5Nb2O9 (NBN-LCN) ceramics. More encouragingly, the system has exceptional thermal stability and is nonsusceptible to mechanical loading. This study not only demonstrates that the high-performance and robust NBN-LCN high-temperature piezoceramics hold great potential for implements under harsh conditions but also opens an avenue for integrating antagonistic properties for the enhancement of the collective performance in functional materials.

Composition Regulation of Potassium Sodium Niobate Thin Films through Post-Annealing under Alkali Element Atmospheres.

Amorphous potassium sodium niobate (KNN) films were synthesized at 300 °C through the radio frequency magnetron sputtering method and subsequently crystallized by post-annealing at 700 °C in various alkali element atmospheres (Na and K). The as-deposited film is notably deficient in alkali metal elements, particularly K, whereas the loss of alkali elements in the films can be replenished through annealing in an alkali element atmosphere. By adjusting the molar ratio of Na and K in the annealing atmosphere, the ratio of Na/K in the resultant film varied, consequently suggesting the efficiency of this method on composition regulation of KNN films. Meanwhile, we also found that the physical characteristics of the films also underwent differences with the change of an annealing atmosphere. The films annealed in a high Na atmosphere exhibit large dielectric losses with limited piezoelectric vibration behavior, while annealing in a high K atmosphere reduces the dielectric losses and enhances the piezoelectric behavior. Furthermore, the results of vibration measurement demonstrated that the film annealed in a mixed powder of 25% Na2CO3 and 75% K2CO3 exhibits an optimal vibration displacement of ~400 pm under the sinusoidal excitation voltage of 8 V. This approach of altering the composition of KNN films through post-annealing may introduce the new concept of property design of KNN as well as other similar films.

Significantly Enhanced Electrostrain in Oriented Epitaxial Self-Assembled Aurivillius-Type Piezoelectric Films via Regulating Polarization Vectors.

High-temperature piezoelectric films with excellent piezoelectric and ferroelectric properties lay the foundation for the development of high-temperature piezo-MEMS devices. However, due to the poor piezoelectricity and strong anisotropy, it remains a challenge to obtain high quality Aurivillius-type high-temperature piezoelectric films with high performance, which impedes their practical implements. Here, a feasible polarization vector regulation strategy associated with oriented epitaxial self-assembled nanostructures for enhancing electrostrain is proposed. Guided by lattice matching relation, non-c-axis oriented epitaxial self-assembled Aurivillius-type calcium bismuth niobate (CaBi2Nb2O9, CBN) high-temperature piezoelectric films were successfully prepared on different oriented Nb-STO substrates. By the lattice matching relationship, hysteresis measurement, and piezoresponse force microscopy analysis, it is confirmed that the polarization vectors transform from a two-dimensional plane to a three-dimensional space, and the out-of-plane polarization switching is enhanced. A platform for more possible polarization vectors is provided in the self-assembled (013)CBN film. More importantly, enhanced ferroelectric (Pr ∼ 13.4 µC/cm2) and large strain (∼0.24%) were obtained in the (013)CBN film, which promotes the great application prospect of CBN piezoelectric films in high-temperature MEMS devices.

Piezoelectric Materials and Sensors for Structural Health Monitoring: Fundamental Aspects, Current Status, and Future Perspectives.

Structural health monitoring technology can assess the status and integrity of structures in real time by advanced sensors, evaluate the remaining life of structure, and make the maintenance decisions on the structures. Piezoelectric materials, which can yield electrical output in response to mechanical strain/stress, are at the heart of structural health monitoring. Here, we present an overview of the recent progress in piezoelectric materials and sensors for structural health monitoring. The article commences with a brief introduction of the fundamental physical science of piezoelectric effect. Emphases are placed on the piezoelectric materials engineered by various strategies and the applications of piezoelectric sensors for structural health monitoring. Finally, challenges along with opportunities for future research and development of high-performance piezoelectric materials and sensors for structural health monitoring are highlighted.

Identifying the Interfacial Polarization in Non-stoichiometric Lead-Free Perovskites by Defect Engineering.

Recent advances in perovskite ferroelectrics have fostered a host of exciting sensors and actuators. Defect engineering provides critical control of the performance of ferroelectric materials, especially lead-free ones. However, it remains a challenge to quantitatively study the concentration of defects due to the complexity of measurement techniques. Here, a feasible approach to analyzing the A-site defect and electron in alkali metal niobate is demonstrated. The theoretical relationships among defect concentration, conductivity, and oxygen partial pressure can be established based on the defect chemistry equilibria. The type and concentration of defects are reflected through the conductivity variation with oxygen partial pressure. As a result, the variation of defect concentration gives rise to defect-driven interfacial polarization, which further leads to distinct properties of the ceramics. e.g., abnormal dielectric behavior. Furthermore, this study also suggests a strategy to manipulate defects and charges in perovskite oxides for performance optimization.

Deciphering the phase transition-induced ultrahigh piezoresponse in (K,Na)NbO3-based piezoceramics.

Here, we introduce phase change mechanisms in lead-free piezoceramics as a strategy to utilize attendant volume change for harvesting large electrostrain. In the newly developed (K,Na)NbO3 solid-solution at the polymorphic phase boundary we combine atomic mapping of the local polar vector with in situ synchrotron X-ray diffraction and density functional theory to uncover the phase change and interpret its underlying nature. We demonstrate that an electric field-induced phase transition between orthorhombic and tetragonal phases triggers a dramatic volume change and contributes to a huge effective piezoelectric coefficient of 1250 pm V-1 along specific crystallographic directions. The existence of the phase transition is validated by a significant volume change evidenced by the simultaneous recording of macroscopic longitudinal and transverse strain. The principle of using phase transition to promote electrostrain provides broader design flexibility in the development of high-performance piezoelectric materials and opens the door for the discovery of high-performance future functional oxides.

Isolated-Oxygen-Vacancy Hardening in Lead-Free Piezoelectrics.

Defect engineering is a well-established approach to customize the functionalities of perovskite oxides. In demanding high-power applications of piezoelectric materials, acceptor doping serves as the state-of-the-art hardening approach, but inevitably deteriorates the electromechanical properties. Here, a new hardening effect associated with isolated oxygen vacancies for achieving well-balanced performances is proposed. Guided by theoretical design, a well-balanced performance of mechanical quality factor (Qm ) and piezoelectric coefficient (d33 ) is achieved in lead-free potassium sodium niobate ceramics, where Qm increases by over 60% while d33 remains almost unchanged. By atomic-scale Z-contrast imaging, hysteresis measurement, and quantitative piezoresponse force microscopy analysis, it is revealed that the improved Qm results from the inhibition of both extrinsic and intrinsic losses while the unchanged d33 is associated with the polarization contributions being retained. More encouragingly, the hardening effect shows exceptional stability with increasing vibration velocity, offering potential in material design for practical high-power applications such as pharmaceutical extraction and ultrasonic osteotomes.

Multiscale structural engineering of dielectric ceramics for energy storage applications: from bulk to thin films.

Dielectric capacitors with the prominent features of ultrafast charging-discharging rates and ultrahigh power densities are ubiquitous components in modern electronics. To meet the growing demand for electronics miniaturization, dielectric capacitors with high energy storage properties are extensively researched. Here we present an overview of the recent progress in the engineering of multiscale structures of dielectric ceramics ranging from bulk to thin films. This article commences with a brief introduction of the fundamentals of dielectric ceramics, including primary parameters, a library of dielectric ceramics, and multiscale structures. Emphases are placed on the relationship between multiscale structures and energy storage properties and the rational structure design principles in dielectric ceramics. Also included are currently available multilayer ceramic capacitors based on multiscale engineered ceramic structures. Finally, challenges along with opportunities for further research and development of high-performance dielectric ceramics for electrostatic energy storage are highlighted.

Refreshing Piezoelectrics: Distinctive Role of Manganese in Lead-Free Perovskites.

Driven by an ever-growing demand for environmentally compatible materials, the past two decades have witnessed the booming development in the field of piezoelectrics. To maximally explore the potential of lead-free piezoelectrics, chemical doping could be an effective approach, referenced from tactics adopted in lead-based piezoelectrics. Herein, we reveal the distinct role of manganese in a promising lead-free perovskite (K, Na)NbO3 (denoted by KNN) in comparison to that in market-dominating lead-based counterparts [Pb(Zr, Ti)O3, PZT]. In contrast to the scenario in PZT, manganese doping in KNN results in tremendously improved piezoelectric coefficient d33 by nearly 200%, whereas the same doping species in PZT deteriorates the d33 down to less than 30% of its original value. The result is rationalized from macroscopic and local electrical characterizations down to atomic-scale visualization. This study demonstrates that there is enormous space to further enhance piezoelectricity in lead-free systems because the chemical doping effect may completely differ in lead-containing and lead-free perovskites.

The effect of Cu substitution on microstructure and thermoelectric properties of LaCoO3 ceramics.

La(Co, Cu)O(3-δ) ceramics were prepared by pressureless sintering of citrate precursor powders, and their thermoelectric properties were investigated with an emphasis on the influence of Cu doping and phase structure as well as microstructure. It was found that a secondary phase first appeared in the form of a network along the grain boundaries and then changed to dispersion with increasing Cu content, which effectively reduced the lattice thermal conductivity of the materials. The thermal conductivity was only 1.21 W m(-1) K(-1) for the sample LaCo(0.75)Cu(0.25)O(3-δ), being much lower as for the thermoelectric oxide materials. In addition, a small amount of Cu substitution for Co increased the electrical conductivity greatly and the absolute Seebeck coefficient, whose sign was also reversed from negative to positive. The dimensionless figure of merit, ZT, of LaCoO(3-δ) oxides at low and middle temperatures can be remarkably enhanced by substituting Co with Cu.