Engineering Multiphase Phase Transitions for Exceptional Electrocaloric Performance and Ultraweak Electrostrictive Response in Ferroelectrics.

In the pursuit of eco-friendly alternatives for refrigeration technology, electrocaloric materials have emerged as promising candidates for efficient solid-state refrigeration due to their high efficiency and integrability. However, current advancements in electrocaloric effects (ECEs) are often constrained by high temperatures and elevated electric fields (E-field), limiting practical applicability. Informed by phase-field simulation, this study introduces a (1-x)Pb(Yb1/2Nb1/2)O3-xPb(Mg1/3Nb2/3)O3 system, strategically engineered to incorporate highly ordered YN and disordered MN mixtures. The synergistic interplay between E-field/temperature-induced polarization reorientation and cation shift initiates multiple ferroelectric-antiferroelectric-paraelectric phase transitions. Our results demonstrate that under a moderate E-field of 50 kV cm-1, the x = 0.22 composition achieves remarkable performance with a giant temperature change (ΔT) of 3.48 K, a robust ECE strength (ΔT/ΔE) of 0.095 K cm kV-1, and a wide temperature span (Tspan) of 38 °C. Notably, the disrupted lattice structure contributes to ultralow electrostrains below 0.008%, with an average electrostrictive coefficient Q33 of 0.007 m4 C-2. The significantly weakened electrostrictive activity favors enhancing the performance stability of subsequent devices. This work introduces an innovative strategy for developing robust electrocaloric materials, offering substantial ΔT and low electrostrains, presenting promising advancements in ECE applications with an extended lifetime.

Ultra-Weak Polarization-Strain Coupling Effect Boosts Capacitive Energy Storage.

In pulse power systems, multilayer ceramic capacitors (MLCCs) encounter significant challenges due to the heightened loading electric field (E), which can lead to fatigue damage and ultrasonic concussion caused by electrostrictive strain. To address these issues, an innovative strategy focused on achieving an ultra-weak polarization-strain coupling effect is proposed, which effectively reduces strain in MLCCs. Remarkably, an ultra-low electrostrictive coefficient (Q33) of 0.012 m4 C-2 is achieved in the composition 0.55(Bi0.5Na0.5)TiO3-0.45Pb(Mg1/3Nb2/3)O3, resulting in a significantly reduced strain of 0.118% at 330 kV cm-1. At the atomic scale, the local structural heterogeneity leads to an expanded and loose lattice structure, providing ample space for large ionic displacement polarization instead of lattice stretching when subjected to the applied E. This unique behavior not only promotes energy storage performance (ESP) but also accounts for the observed ultra-low Q33 and strain. Consequently, the MLCC device exhibits an impressive energy storage density of 14.6 J cm-3 and an ultrahigh efficiency of 93% at 720 kV cm-1. Furthermore, the superior ESP of the MLCC demonstrates excellent fatigue resistance and temperature stability, making it a promising solution for practical applications. Overall, this pivotal strategy offers a cost-effective solution for state-of-the-art MLCCs with ultra-low strain-vibration in pulse power systems.

Innovative Design of BNKT-xSLZT Ceramics: Maximizing the Polarization Difference for Enhanced Energy Storage.

Lead-free relaxor ferroelectric ceramics with outstanding energy-storage (ES) density (Wrec) and high ES efficiency (η) are crucial for advanced pulse-power capacitors. This study introduces a strategic approach to maximizing the polarization difference (ΔP) by inducing a transition from the ferroelectric phase to the ergodic relaxor (ER) phase. By employing this strategy, a series of ceramics, (1 - x)(Bi0.5Na0.4K0.1)TiO3-x(Sr0.85La0.1)(Zr0.5Ti0.5)O3 (BNKT-xSLZT), with varying SLZT content (x = 0.05, 0.10, 0.15, and 0.20), were designed. The addition of SLZT enhances cationic disorder, induces vacancies at A sites, and disrupts long-range ferroelectric order, facilitating the formation of polar nanoregions and enhancing relaxor ferroelectric behavior. Furthermore, a viscous polymer process (VPP) technology is employed to optimize the ceramics' structure, aiming to increase the breakdown strength (Eb) and enhance ΔP. Ultimately, enhanced ES performance is demonstrated in BNKT-0.15SLZTVPP, achieving a remarkable Wrec of 6.85 J/cm3 and η of 84% under 470 kV/cm. This composition demonstrates excellent stability with minimal variations in Wrec (3.0%) and η (4.4%) over the temperature range of 20-110 °C. Additionally, BNKT-0.15SLZTVPP exhibits exceptional pulse charge-discharge properties, featuring a high discharge density of 3.72 J/cm3, a large power density of 164.2 MW/cm3, and a short discharge time (t0.9) of 193 ns under 300 kV/cm. The study validates the practicality of BNKT-0.15SLZTVPP for pulse capacitors and underscores the potential to enhance ES performance through A-site donor doping and VPP technology. This work provides a comprehensive understanding of the interplay among composition, structure, and ES properties in lead-free relaxor dielectric ceramics, laying the groundwork for innovative advancements in the field.

Moderate Fields, Maximum Potential: Achieving High Records with Temperature-Stable Energy Storage in Lead-Free BNT-Based Ceramics.

The increasing awareness of environmental concerns has prompted a surge in the exploration of lead-free, high-power ceramic capacitors. Ongoing efforts to develop lead-free dielectric ceramics with exceptional energy-storage performance (ESP) have predominantly relied on multi-component composite strategies, often accomplished under ultrahigh electric fields. However, this approach poses challenges in insulation and system downsizing due to the necessary working voltage under such conditions. Despite extensive study, bulk ceramics of (Bi0.5Na0.5)TiO3 (BNT), a prominent lead-free dielectric ceramic family, have seldom achieved a recoverable energy-storage (ES) density (Wrec) exceeding 7 J cm-3. This study introduces a novel approach to attain ceramic capacitors with high ESP under moderate electric fields by regulating permittivity based on a linear dielectric model, enhancing insulation quality, and engineering domain structures through chemical formula optimization. The incorporation of SrTiO3 (ST) into the BNT matrix is revealed to reduce the dielectric constant, while the addition of Bi(Mg2/3Nb1/3)O3 (BMN) aids in maintaining polarization. Additionally, the study elucidates the methodology to achieve high ESP at moderate electric fields ranging from 300 to 500 kV cm-1. In our optimized composition, 0.5(Bi0.5Na0.4K0.1)TiO3-0.5(2/3ST-1/3BMN) (B-0.5SB) ceramics, we achieved a Wrec of 7.19 J cm-3 with an efficiency of 93.8% at 460 kV cm-1. Impressively, the B-0.5SB ceramics exhibit remarkable thermal stability between 30 and 140 °C under 365 kV cm-1, maintaining a Wrec exceeding 5 J cm-3. This study not only establishes the B-0.5SB ceramics as promising candidates for ES materials but also demonstrates the feasibility of optimizing ESP by modifying the dielectric constant under specific electric field conditions. Simultaneously, it provides valuable insights for the future design of ceramic capacitors with high ESP under constraints of limited electric field.