Multilayer ceramic capacitors (MLCCs) have become the core materials in advanced electronics and power equipment thanks to the excellent functional characteristics, including energy storage, filtering, and coupling. However, the next-generation electronic devices place higher demands on the energy storage performance for MLCCs. This study demonstrates that the directional regulation of gradient polarization coupling (GPC) constitutes an effective approach to achieving a giant energy storage density. With the guidance of theoretical predictions, we propose a high configurational entropy (HCE) strategy in NaNbO3-based (NN) multilayer ceramic capacitors to constructing the alternating multipolar nanodomains. Alternately distributed weakly polar and strongly polar domains with embedding nonpolar nanoclusters possess the effective gradient coupling of polarization. Polymorphic polarization coupling realizes the dynamic orientation of local nanoclusters to drive the orientation of the overall electric dipoles, which could reduce hysteresis loss while maintaining high polarization strength. As a consequence, the NN-20H MLCCs achieve a recoverable energy storage density of 20.4 J/cm3 and an ultrahigh breakdown strength of 1680 kV/cm, which demonstrates great advancement in reported lead-free ceramic capacitors. This work illustrates the GPC strategy to advance novel insights for next-generation MLCCs with high energy storage performance.

Overcoming the trade-off between multiphase coexistence and phase transformation in piezoelectrics remains a critical challenge for achieving high and stable piezoelectric performance over a broad temperature range. Here, we resolve this long-standing dilemma by constructing a continuous phase transition through multilayer ceramic texture engineering. Specifically, two types of (K,Na)NbO3-based piezoelectric ceramics with distinct polymorphic phase boundary (PPB) features are physically composed. The composite ceramics exhibit hierarchic phase and domain structures, particularly a continuous phase transition, enabling outstanding piezoelectric performance and thermal stability across a wide temperature range. As a result, the multilayer composite ceramics prepared in this work demonstrate excellent room-temperature piezoelectric properties, with a piezoelectric coefficient (d33) ∼ 420 pC N-1 and an inverse piezoelectric coefficient (d33*) ∼ 600 pm V-1. More importantly, within the temperature range of 25°C-100°C, the variation in d33 and d33* values is merely 2%. This work establishes a continuous phase transition-driven paradigm for enhancing piezoelectric thermal stability, demonstrating universal potential to decouple the constraints imposed by multiphase coexistence and phase transformation in next-generation piezoelectric materials.

Antiferroelectrics, distinguished by antipolar ordering configurations, have emerged as prime candidates for advanced energy-storage systems due to their near-zero remnant polarization and elevated field-induced maximum polarization. However, the trade-off between high recoverable energy density and high efficiency remains a major challenge in antiferroelectric ceramics. Here, guided by phase-field simulations, we propose a new strategy, namely antipolar-breaking, by disordering dipoles within a 4-fold antiferroelectric modulation framework, resulting in tuned phase-transition fields and simultaneously reduced hysteresis loss. Leveraging this strategy, an ultrahigh recoverable energy density of 23.8 J cm-3 and an excellent efficiency of 93.1% are achieved in PbZrO3-based antiferroelectric ceramics, surpassing state-of-the-art ceramic dielectrics. Atomic-level imaging and dynamical simulations reveal that localized compositional fluctuations induce anti-polar-breaking sites, attenuating long-range antiferroelectric interactions and precisely controlling polarization evolution, thereby improving comprehensive energy storage. This strategy opens up a new avenue to manipulate the antiferroelectric-ferroelectric phase-transition path and acquire high-performance energy storage in antiferroelectrics.

Lead-free capacitor ceramics offer substantial advantages in the latest generation of power devices owing to their outstanding energy storage capabilities. However, their relatively low energy storage density has hindered the progress of ceramic capacitors. Consequently, the energy storage performance was enhanced by introducing Na0.5Bi0.5TiO3 into BaTiO3, forming relaxor ferroelectrics. Sr(Al0.5Nb0.5)O3 was incorporated to disrupt longrange ordered ferroelectric domains, thereby modifying its domain structure and microscopic morphology. This process culminates in a high efficiency (eta) of 92.4 % and a substantial recovered energy density (Wrec) of 7.5 J cm-3. The material also demonstrates excellent temperature stability within the range of 25-200 degrees C, with a Wrec of 2.9 f 0.1 J cm-3. Furthermore, it exhibits frequency stability spanning from 1 to 200 Hz, with a Wrec of 2.9 f 0.1 J cm-3. Notably, displays cycle stability of Wrec at 2.8 f 0.1 J cm-3 with an electric field of 300 kV cm-1. The present study presents a method for the fabrication of lead-free ferroelectric ceramics with high-power-density energy storage capacitors. This methodology involves optimizing composition and engineering domain size.

Dielectric capacitors represent a promising alternative to conventional electrochemical counterparts for applications in high-voltage networks, integrated circuits, and portable flexible electronics. Currently, most practical dielectric polymers are derived from petroleum-based sources, whereas environmentally sustainable biomass dielectric materials remain largely underexplored. We report a class of cyanoethyl cellulose (CEC)-based nanocomposites enhanced with polyethyleneimine-based polymer dots (PEPDs), which simultaneously elevate both the dielectric constant (epsilon r) and breakdown strength (Eb). The wide-band-gap PEPDs with abundant amino groups form hydrogen bonds with the CEC backbone, ensuring uniform dispersion and creating continuous polar interfacial regions that substantially improve epsilon r. In parallel, the high electron affinity of the polymer matrix, together with deep-level traps introduced by the wide-band-gap PEPDs, effectively suppresses charge migration and reduces conductive loss, leading to a notable enhancement in Eb. As a result, the optimized composite achieves a remarkable discharged energy density (Ud) of 35.2 J cm-3 at 700 MV m-1, outperforming current dielectric biomass materials. This work establishes a promising pathway for the development of cellulose-based nanocomposites toward next-generation high-energy-density dielectric capacitors.

Developing dielectric capacitors with robust energy storage capabilities across a broad temperature range, especially in high-temperature environments, remains a formidable challenge in cutting-edge advanced power and electronic systems. The complexity arises from the evolving lattice symmetry and the accompanying changes in dielectric polarization as the temperature fluctuates, making it challenging to maintain consistently high and stable energy storage performance at high temperature. By leveraging first-principles calculations, we propose a novel strategy that intergrates entropy modulation with crystal symmetry phase shifting. This approach triggers ordered-disordered transitions and a shift from low to high symmetry at ambient temperature, thereby enhancing the polarization response, improving insulating properties, and expanding the temperature range for the highsymmetry phase to exist. Remarkably, our Bi0.5Na0.5TiO3-based high-entropy thin film capacitor not only showcases industry-leading energy storage properties at room temperature, with a recoverable energy storage density of 103 J cm-3, but also extends its stable operating temperature range to an ultra-high level of 320 degrees C. This innovative method paves the way for advancement in high-temperature dielectric energy storage capacitors.

The urgent need to develop polymer dielectrics with high energy storage density (Ue) has become paramount to fulfill the requirements of cutting-edge electrical and electronic systems. Here, ultralow nano-hierarchical filler loadings were introduced to enhance the Ue and efficiency (eta) of polyethermide (PEI) over a broad temperature. The nano-hierarchical structure is constructed by loading with barium titanate nanoparticles (BTNPs) on boron nitride nanosheets (BNNSs), and then coating with an Al2O3 insulating layer around BT@BN fillers. Experiment results in conjunction with simulations demonstrate that the ultra-low BT@BN filler loadings are to enhance the maximum electrical displacement (Dmax) and breakdown strength (Eb) of nanocomposites, while the Al2O3 layer are coated on the BT@BN nanofillers to further mitigate the pronounced interfacial polarization effect between BTNPs and PEI matrix, resulting higher Dmax and Eb of nanocomposites. More importantly, benefitting the high thermal conductivity of BNNSs and the generated trap energy levels of BNNSs and Al2O3 with wide band gap, both the energy efficiency (Ue) and eta are significantly enhanced at high temperatures. Specifically, when the filler content was 0.75 wt%, the Ue and eta of nanocomposites are 10.66 J/cm3 and 93.30 % (@RT), 3.11 J/cm3 and 81.45 % (@200 degrees C). This work offers a good example for the design and development of polymer dielectrics for applications over a wide temperature range.

Multiphase transition type antiferroelectric lead zirconate is one of the ideal candidate dielectrics for energy storage ceramic capacitors, it is challenging to fully reveal its formation and regulation mechanism, and further enhance the energy storage performance. Here, the essence of polymorphic modulation of multiphase transition antiferroelectric is proposed, and its non-ergodic relaxor phase transition nature is revealed. The polymorphic modulated antiferroelectric ceramics show a giant energy storage density of 23.73 J cm-3 and an excellent efficiency of 88%, which is much superior to the commensurate and incommensurate modulated antiferroelectric phases and other dielectric ceramics. The polymorphic modulated antiferroelectric ceramic is composed of both commensurate and incommensurate modulated ferrielectric like antiferroelectric sub-grain regions. Under an electric field, relaxor ferroelectric and ferroelectric phases are successively derived from the incommensurate and commensurate antiferroelectric regions, constituting two distinct non-ergodic relaxor ferroelectric states. The independent evolution of antiferroelectric short-range to ferroelectric short-range and ferroelectric long-range, and their interaction are the key to the excellent energy storage performance of polymorphic modulated antiferroelectric ceramics. The findings offer a novel insight into the field-induced phase transition in antiferroelectric, and promote the potential applications of pulse power antiferroelectric ceramic capacitors.

Dielectric capacitors with high energy storage performance are highly desired for advanced power electronic devices and systems. Even though strenuous efforts have been dedicated to closing the gap of energy storage density between the dielectric capacitors and the electrochemical capacitors/batteries, a single-minded pursuit of high energy density without a near-zero energy loss for ultrahigh energy efficiency as the grantee is in vain. Herein, for the purpose of decoupling the inherent conflicts between high polarization and low electric hysteresis (loss), and achieving high energy storage density and efficiency simultaneously in multilayer ceramic capacitors (MLCCs), we propose an interlaminar strain engineering strategy to modulate the domain structure and manipulate the polarization behavior of the dielectric mediums. With a heterogeneous layered structure consisting of different antiferroelectric ceramics [(Pb0.9Ba0.04La0.04)(Zr0.65Sn0.3Ti0.05)O3/(Pb0.95Ba0.02La0.02)(Zr0.6Sn0.4)O3/(Pb0.92Ca0.06La0.02)(Zr0.6Sn0.4)0.995O3], our MLCC exhibits a giant recoverable energy density of 22.0 J cm-3 with an ultrahigh energy efficiency of 96.1%. Combined with the favorable temperature and frequency stabilities and the high antifatigue property, this work provides a strain engineering paradigm for designing MLCCs for high-power energy storage and conversion systems.

A novel nanoplex-driven architecture was constructed that integrated short-range ordered antiferroelectric nanodomains with highly disordered relaxor ferroelectrics.

Along with the progress of Artificial Intelligence and the network technology, there are higher requirements for load sensing and vibration control, which has driven the growth of demand for high-performance piezoelectric ceramic components. Although continuous breakthroughs have been implemented to unilaterally improve the piezoelectricity in recent years, achieving high electromechanical plane coupling coefficient (k(p)), Curie temperature (T-C) along with a high piezoelectric coefficient (d(33)) remains a major challenge. To address the mutual limitation between these parameter, this work employs the template grain growth technique combined with the stepwise chemical modification strategy to prepare (K0.5Na0.5)NbO3-based (KNN) textured ceramics with Orthorhombic-Tetragonal (O-T) phase boundary characteristics. The results indicate that the optimized 0.98((K0.5Na0.5)(Nb0.98Ta0.02)O-3)-0.01(Bi(Ni0.67Nb0.33)O-3)-0.01(Bi0.5K0.5)HfO3-3wt%NaNbO3 (abbreviated as T-1BKH) ceramics achieved high electrical coefficient (d(33) similar to 505 pC/N) and outstanding electromechanical coupling coefficient (k(p) similar to 72 %) while maintaining a superior Curie temperature (T-C similar to 377 degrees C), which offer highly competitive among lead-free piezoelectric ceramics. More importantly, it can exhibit high output power density (P-D similar to 10.7 mW/cm(3)) when making piezoelectric circular diaphragm energy harvesters. This work not only provides important guidance for the synergistic regulation among crystal orientation and phase boundaries of the comprehensive piezoelectricity of KNN-based ceramics, but also promotes the study of its application.

Overcoming the polarization‐relaxor trade‐off in dielectric capacitors remains a critical challenge for achieving simultaneous high energy density ( W rec ) and efficiency ( η ). While conventional polar nano‐regions (PNRs) enhance relaxor behavior, their limited dipole vector lengths inevitably suppress polarization strength. Here, the long‐standing dilemma is resolved by constructing topological vortex domains (VDs) within PNRs (VPNR) through synergistic disorder engineering and grain size confinement in BiFeO 3 ‐based thin films. Phase‐field simulations reveal that the VPNR structure combines ultralow domain‐switching energy barriers with minimally reduced polarization vectors under high electric fields, enabling concurrent optimization of relaxor dynamics and polarization strength. Experimental validations via multiscale characterization confirm that the engineered VPNR configuration exhibits balanced polarization characteristics of high maximum polarization and small remanent polarization. The optimized film achieves a breakthrough W rec of 130 J cm −3 and η of 80% at 4864 kV cm −1 , surpassing pristine BiFeO 3 by 545% and 400%, respectively. This work establishes a topology‐driven paradigm for dielectric energy storage, demonstrating universal potential to decouple polarization‐relaxor constraints in next‐generation capacitive materials.

Antiferroelectric ceramics, driven by electric-field-induced antiferroelectric-ferroelectric phase transitions, hold exceptional potential for high capacitance density capacitors. However, conventional antiferroelectric ceramics are capable of releasing only 70-80% of the energy during the charging-discharging cycles, limiting their practical applications. Herein, we propose a novel approach using heterogeneous dipolar structures in PbHfO3-based AFE ceramics to achieve remarkable energy density. By compositionally inducing structural order-disorder transitions, heterogeneous dipolar structures with complex interactions are created, within which dipoles can rapidly flip under the applied electric field, thereby substantially reducing the hysteresis losses. Combined with significantly improved breakdown strength, the optimized antiferroelectric ceramics exhibits a large recoverable energy density approximately 20.04 J cm-3 and a high efficiency of around 90.5%, setting a new benchmark for antiferroelectric ceramics. This work, focusing on the atomic scale, clarifies the structure-property relationship and provides valuable insights for developing next-generation high-performance antiferroelectric materials.

Combining layers with high breakdown resistance and high polarization is a promising approach for designing dielectric capacitors with high energy density and efficiency. However, such combinations often accompany strong interfacial polarization, magnification of local electric fields, leading to premature breakdown. This work addresses this issue via controlled formation of diffusospheres. We constructed multilayer heterogeneous films using two Bi0.5Na0.5TiO3 (BNT)-based substances with high breakdown resistance and high polarization properties. Experimental results and finite element simulations demonstrate that the energy storage capacity of these films effectively harnesses the advantages of both phases. Notably, the interface polarization is minimal. Instead, a solid solution-like diffusosphere, formed by the mutual diffusion of ions between the two phases, plays a crucial role. The diffusosphere acts as a transition zone, mitigating charge aggregation at the interfaces and optimizing the relaxor and breakdown characteristics of the capacitor. With six diffusospheres, the multilayer heterogeneous capacitor achieves a recoverable energy storage density of 94 J/cm3, a significant advancement in BNT-based energy storage films. This work proposes and validates the concept of diffusospheres and their role in reducing interfacial polarization in multilayer heterogeneous films, enhancing the understanding of heterogeneous composite structures and advancing the field of dielectric energy storage.

Pulsed power systems urgently demand dielectric materials with superior energy storage density (W-rec) and charge-discharge efficiency (eta). However, achieving concurrent high W-rec and eta in lead-free ceramics remains challenging due to polarization hysteresis and early saturation issues. Here, we propose a nano-domain engineering strategy to reconfigure the energy-storage in NaNbO3(NN)-based relaxor ferroelectrics. The doping of Bi3+ and Ta5+ induces lattice distortion and disorder, disrupting the antiferroelectric (AFE) structure for a ferroelectric (FE) state. Additionally, incorporating Sr0.7Bi0.2TiO3 optimizes relaxor characteristics, stabilizing FE Q-phase with nano-domains. Optimized ceramics exhibit ultrahigh energy-storage performance among lead-free systems: a W-rec of 10.17 J/cm(3) with eta of 90.06 %, coupled with ultrafast discharge characteristics (W-d similar to 4.81 J/cm(3), P-d similar to 752.03 MW/cm(3)). These findings not only establish NN-based ceramics as promising candidates for advanced energy storage capacitors, but also provide a viable design paradigm for developing high-performance lead-free dielectric materials.

BiFeO3-based ceramics are one of the potential materials expected to replace conventional Pb(Zr,Ti)O3-based ceramics in the field of high-temperature piezoelectricity due to their high Curie temperature (TC). However, the low piezoelectric properties of BiFeO3-based ceramics limit their further development and applications. Here, a synergistic tuning strategy is proposed to enhance the piezoelectric properties of BiFeO3-based ceramics by adjusting the phase configuration near morphotropic phase boundary (MPB) and introducing lattice distortion. Near the MPB, the increased occupation of the T-phase can reduce the domain switch barrier, thereby allowing the dipole to switch more efficiently. Furthermore, enhancing the lattice distortion can increase the intrinsic polarization of ceramics. The above two points serve to enhance the piezoelectric properties of BiFeO3-based ceramics. As a result, 0.7BiFeO3-0.29BaTiO3-0.01Bi0.5K0.5Ti0.5Hf0.5O3 ceramics possesses a high piezoelectric coefficient d33 of 198 f 5 pC/N, and a high TC of 489 f 6 degrees C, while maintaining stable performance across a broad temperature range from 25 to 404 degrees C. This synergistic modulation strategy provides an idea to optimize the piezoelectric properties of BiFeO3-based ceramics for high-temperature applications.

Enhancing the piezoelectric or strain response of materials through nanodomain engineering has proven to be highly effective. Here, we demonstrate that topological bubble domains (BDs) can be induced in Bi 0.5 Na 0.5 TiO 3 (BNT)–based thin films via lattice distortions. We establish a positive correlation between the density of BDs, macroscopic polarization, and strain response. The BDs in BNT-based thin films leads to a remarkable enhancement in the strain response, reaching ~400% of the virgin state. This enhancement arises from the lower energy barriers for dipole flipping and domain switching associated with BDs, in comparison to conventional domain structures. Under an applied electric field, the rotation of polarized BDs, combined with a reduction in dipole flux due to the articulated rotation between BDs and surrounding domains, further amplifies the strain response. These findings advance our understanding of BDs in electromechanical materials and provide theoretical guidance for designing high-performance piezoelectrics with polar topologies.

Commensurate modulated antiferroelectric ceramics exhibit limited application prospects, a quasi transient antiferroelectric-ferroelectric phase transition has locked their energy storage performance. Highly homogeneous oxygen octahedra set produce only one type of antiferrodistortion-ferrodistortion transition, followed by a rapid triggering of the antiferroelectric-ferroelectric phase transition. Here, we propose a strategy of structural order differentiation engineering to disrupt the homogeneity of oxygen octahedra by initiator/enhancer co-substitution, and we have successfully unlocked the energy storage performance of commensurate modulated antiferroelectric ceramics. By constructing oxygen octahedra sets with highly differentiated rotational distortions, an energy storage density of 23.11 J/cm3, an energy storage efficiency of 85.55%, and a discharge energy density of up to 16.45 J/cm3 are simultaneously achieved, which is superior to other antiferroelectric ceramics and dielectric ceramics. By limiting the doping window, the commensurate modulation characteristics of polarization order can be maintained, which ensures the maximum polarization. A highly differentiated octahedra rotational distortion yields a multi-stage antiferrodistortion-ferrodistortion transition and a coexistence of polymorphic ferroelectric phases, significantly prolonging the polarization process. The proposed structural order differentiation shows guiding significance for the development of antiferroelectric, and the obtained energy storage performance promotes the practical applications of antiferroelectric ceramic capacitors.

Antiferroelectric (AFE) ceramics are known for their rich field-induced phase transitions, which mainly contribute to their superior energy storage performance. However, the phase transitions instability caused by high temperature often limits its application scenarios. Developing AFE ceramics with high energy storage properties and wide application temperature ranges is challenging. Here, considering the B-site ordering characteristics of Pb(Yb0.5Nb0.5)O3, we propose a simple approach for introducing A-site distortion and adjusting Bsite ordering to confront these challenges. In our Fe3+/Sr2+co-doping system, we realized an ultra-wide temperature range of 25-200 degrees C, within which the recoverable storage density was considerable: 8.48-13.39 J cm- 3. In this interval, the discharge energy density could reach 6.15-9.67J cm-3, and the discharge current density and discharge power density were 755.09-1667.36 A cm- 2 and 207.65-500.21 MW cm-3, respectively. The obtained high-temperature energy storage performance was superior to that of existing energy storage ceramics or polymer films. The introduction of A-site distortion improves the stability of AFE phase, the decrease in B-site ordering suppresses the remanent polarization and delays change in structural symmetry with temperature. This study forms a basis for further applications of dielectric capacitors and signifies the development of widetemperature-range energy storage devices.

Eco-friendly NaNbO3 (NN)-based relaxor ferroelectric ceramics with high dielectric constants cannot meet the high piezoelectric activity quality factors (FOMs: d33 × g33) requirements of electromechanically coupled devices. To solve this issue, we successfully improved the piezoelectricity of NN-based relaxor piezoceramics while reducing the dielectric constant based on microstructural tuning by virtue of the chemical design and texturing engineering. Mainly affected by the highly <001>c orientation and relaxor MPB, the obtained novel 88.5NaNbO3–10Ba(Ti0.7Sn0.3)O3–1.5NaSbO3 texture ceramics enjoys an ultrahigh piezoelectric coefficient (d33 = 423 pC/N), reaching a record high in NaNbO3-based lead-free ceramics. Meanwhile, a large FOMs value (d33 × g33 = 13.3·10−12 m2/N) is successfully realized due to the suppression of the dielectric constant. More importantly, the stable phase/domain evolution also encourages excellent temperature stability for piezoelectricity and FOMs. Especially for the piezoelectricity, when the annealing temperature is < 140 °C, the d33 of the 1.5T ceramics can be stabilized ∼ 400 pC/N. Such excellent electrical temperature stability shows more competition in the reported NN-based piezoceramics. This work not only provides a design paradigm for high-performance piezoelectric materials, but also facilitates their development in electromechanical coupling devices.