Polymorphic Heterogeneous Polar Structure Enabled Superior Capacitive Energy Storage in Lead-Free Relaxor Ferroelectrics at Low Electric Field.

High-performance energy storage dielectrics capable of low/moderate field operation are vital in advanced electrical and electronic systems. However, in contrast to achievements in enhancing recoverable energy density (Wrec), the active realization of superior Wrec and energy efficiency (η) with giant energy-storage coefficient (Wrec/E) in low/moderate electric field (E) regions is much more challenging for dielectric materials. Herein, lead-free relaxor ferroelectrics are reported with giant Wrec/E designed with polymorphic heterogeneous polar structure. Following the guidance of Landau phenomenological theory and rational composition construction, the conceived (Bi0.5Na0.5)TiO3-based ternary solid solution that delivers giant Wrec/E of ≈0.0168 µC cm-2, high Wrec of ≈4.71 J cm-3 and high η of ≈93% under low E of 280 kV cm-1, accompanied by great stabilities against temperature/frequency/cycling number and excellent charging-discharging properties, which is ahead of most currently reported lead-free energy storage bulk ceramics measured at same E range. Atomistic observations reveal that the correlated coexisting local rhombohedral-tetragonal polar nanoregions embedded in the cubic matrix are constructed, which enables high polarization, minimized hysteresis, and significantly delayed polarization saturation concurrently, endowing giant Wrec/E along with high Wrec and η. These findings advance the superiority and feasibility of polymorphic nanodomains in designing highly efficient capacitors for low/moderate field-region practical applications.

Research on Improved Crystallization Properties and Underlying Mechanism of the Sb2Te3 Phase-Change Thin Film by Inserting Sn15Sb85 Layers.

As a non-volatile semiconductor memory technology, phase-change memory has a wide range of application prospects as a result of the excellent comprehensive performance. In this paper, multilayer thin films based on Sb2Te3 material were designed and prepared by inserting the Sn15Sb85 layer. The thermal and electrical properties of superlattice-like Sb2Te3/Sn15Sb85 phase-change films can be adjusted by controlling the thickness ratio of Sb2Te3/Sn15Sb85. In comparison to the monolayer Sb2Te3 film, the multilayer layer Sb2Te3/Sn15Sb85 materials have a higher crystallization temperature, larger crystallization activation energy, and longer data lifetime, indicating the great improvement of thermal stability. The changes in the phase structure and vibrational modes of multilayer Sb2Te3/Sn15Sb85 films were characterized by X-ray diffraction and Raman spectroscopy, respectively. The presence of Sn15Sb85 layers restrains grain growth and refines the grain size. The multilayer Sb2Te3/Sn15Sb85 films exhibit better surface flatness, smaller surface potential undulation, and lower thickness variations than single-layer Sb2Te3. Phase-change memory cells based on the [Sb2Te3 (1 nm)/Sn15Sb85 (9 nm)]5 thin film has a lower threshold voltage (1.9 V) and threshold current (3.1 µA) compared to the Ge2Sb2Te5 film. Meanwhile, the electrical heating model of a phase-change memory cell based on a [Sb2Te3 (1 nm)/Sn15Sb85 (9 nm)]5 multilayer structure was established by multiphysics coupling analysis, proving the great improvement in heat transfer performance and efficiency. The experimental and theoretical studies confirm that the insertion of the Sn15Sb85 layer can significantly improve the crystallization properties of Sb2Te3 films, paving the way for optimizing the phase-change materials by regulating the microstructural parameters.

Achieving Ultrahigh Electrocaloric Response in (Bi0.5Na0.5)TiO3-Based Ceramics through B-Site Defect Engineering.

Lead-free electrocaloric (EC) ferroelectrics are considered ideal for the next generation of environmentally friendly solid-state refrigeration materials. However, their inferior performance compared to lead-based materials significantly restricts their potential application. According to phase-field simulations, it is predicted that the pinning effect of a moderate number of defects can effectively enhance the reversible polarization response associated with the entropy change. Herein, sodium-bismuth titanate (BNT) ceramics with high spontaneous polarization are selected to construct B-site defects by introducing Li+ and Nb5+. Under an electric field of 6 kV mm-1, ultrahigh EC temperature changes of ΔTpos = 1.77 and ΔTneg = 1.49 K are achieved at 65 °C by direct measurement (ΔTneg > 1 K over 55-120 °C). Furthermore, ΔTneg remains above 0.70 K in the temperature range from 25 to 130 °C, exhibiting immense potential for practical applications. This study offers a promising direction for optimizing the EC response in defect systems.

Enhanced Generation of Reactive Oxygen Species via Piezoelectrics based on p-n Heterojunctions with Built-In Electric Field.

Tuning the charge transfer processes through a built-in electric field is an effective way to accelerate the dynamics of electro- and photocatalytic reactions. However, the coupling of the built-in electric field of p-n heterojunctions and the microstrain-induced polarization on the impact of piezocatalysis has not been fully explored. Herein, we demonstrate the role of the built-in electric field of p-type BiOI/n-type BiVO4 heterojunctions in enhancing their piezocatalytic behaviors. The highly crystalline p-n heterojunction is synthesized by using a coprecipitation method under ambient aqueous conditions. Under ultrasonic irradiation in water exposed to air, the p-n heterojunctions exhibit significantly higher production rates of reactive species (·OH, ·O2-, and 1O2) as compared to isolated BiVO4 and BiOI. Also, the piezocatalytic rate of H2O2 production with the BiOI/BiVO4 heterojunction reaches 480 µmol g-1 h-1, which is 1.6- and 12-fold higher than those of BiVO4 and BiOI, respectively. Furthermore, the p-n heterojunction maintains a highly stable H2O2 production rate under ultrasonic irradiation for up to 5 h. The results from the experiments and equation-driven simulations of the strain and piezoelectric potential distributions indicate that the piezocatalytic reactivity of the p-n heterojunction resulted from the polarization intensity induced by periodic ultrasound, which is enhanced by the built-in electric field of the p-n heterojunctions. This study provides new insights into the design of piezocatalysts and opens up new prospects for applications in medicine, environmental remediation, and sonochemical sensors.

Improvement of Multilevel Memory Performance of MnTe Thin Films by Ta Doping.

The pressing need for data storage in the era of big data has driven the development of new storage technologies. As a prominent contender for next-generation memory, phase-change memory can effectively increase storage density through multilevel cell operation and can be applied to neuromorphic and in-memory computing. Herein, the structure and properties of Ta-doped MnTe thin films and their inherent correlations are systematically investigated. Amorphous MnTe thin films sequentially precipitated cubic MnTe2 and hexagonal Te phases with increasing temperature, causing resistance changes. Ta doping inhibited phase segregation in the films and improved their thermal stability in the amorphous state. A phase-change memory cell based on a Ta2.8%-MnTe thin film exhibited three stable resistive states with low resistive drift coefficients. The study findings reveal the possibility of regulating the two-step phase-change process in Ta-MnTe thin films, providing insight into the design of multilevel phase-change memory.

Multiscale reconfiguration induced highly saturated poling in lead-free piezoceramics for giant energy conversion.

The development of high-performance lead-free K0.5Na0.5NbO3-based piezoceramics for replacing commercial lead-containing counterparts is crucial for achieving environmentally sustainable society. Although the proposed new phase boundaries (NPB) can effectively improve the piezoelectricity of KNN-based ceramics, the difficulty of achieving saturated poling and the underlying multiscale structures resolution of their complex microstructures are urgent issues. Here, we employ a medium entropy strategy to design NPB and utilize texture engineering to induce crystal orientation. The developed K0.5Na0.5NbO3-based ceramics enjoys both prominent piezoelectric performance and satisfactory Curie temperature, thus exhibiting an ultrahigh energy harvesting performance as well as excellent transducer performance, which is highly competitive in both lead-free and lead-based piezoceramics. Comprehensive structural analysis have ascertained that the field-induced efficient multiscale polarization configurations irreversible transitions greatly encourages high saturated poling. This study demonstrates a strategy for designing high-performance piezoceramics and establishes a close correlation between the piezoelectricty and the underlying multiscale structures.

Ultrahigh Energy Storage Density and Efficiency of Lead-Free Dielectrics with Sandwich Structure.

Lead-free dielectric capacitors have attracted significant research interest for high-power applications due to their environmental benefits and ability to meet the demanding performance requirements of electronic devices. However, the development of lead-free ceramic dielectrics with outstanding energy storage performance remains a challenge. In this study, environmentally friendly ceramic dielectrics with sandwich structures are designed and fabricated to improve energy storage performance via the synergistic effect of different dielectrics. The chemical compositions of the outer and middle layers of the sandwich structure are 0.35BiFeO3 -0.65SrTiO3 and Bi0.39 Na0.36 Sr0.25 TiO3 , respectively. The experimental and theoretical simulation results demonstrate that the breakdown strength is over 700 kV cm-1 for prepare sandwich structure ceramics. As a result, an ultrahigh recoverable energy storage density of 9.05 J cm-3 and a near-ideal energy storage efficiency of 97% are simultaneously achieved under 710 kV cm-1 . Furthermore, the energy storage efficiency maintains high values (≥ 96%) within 1-100 Hz and the power density as high as 188 MW cm-3 under 400 kV cm-1 . These results indicate that the designed lead-free ceramics with a sandwich structure possess superior comprehensive energy storage performance, making them promising lead-free candidates in the energy storage field.

Tailoring Phase Fraction Induced Saturation Polarization Delay for High-Performance BaTiO3-Based Relaxed Ferroelectric Capacitors.

Electrostatic capacitors based on dielectric materials are essential for enabling technological advances, including miniaturization and integration of electronic devices. However, maintaining a high polarization and breakdown field strength simultaneously in electrostatic capacitors remains a major challenge for industrial applications. Herein, a universal approach to delaying saturation polarization in BaTiO3-based ceramic is reported via tailoring phase fraction to improve capacitive performance. The ceramic of 0.85(0.7BaTiO3-0.3Bi0.5Na0.5TiO3)-0.15Bi0.5Li0.5(Ti0.75Ta0.2)O3 delivers an ultrahigh recoverable energy density (Wrec) of 7.16 J cm-3 along with an efficiency (η) of approximately 90% at a breakdown electric field of 700 kV cm-1, outperforming the current BaTiO3-based ceramics and other lead-free ceramics. Meanwhile, the Wrec and η exhibit wide frequency, temperature, and cycling fatigue stability. Additionally, both an extremely fast discharge time of 115 ns and a large power density of 106.16 MW cm-3 are concurrently attained. This work offers a promising pathway for delaying saturation polarization design in order to create scalable high-energy-density ceramics capacitors and highlight the research prospects of pulse power applications.

Giant Energy Storage Density with Antiferroelectric-Like Properties in BNT-Based Ceramics via Phase Structure Engineering.

Driven by the information industry, advanced electronic devices require dielectric materials which combine both excellent energy storage properties and high temperature stability. These requirements hold the most promise for ceramic capacitors. Among these, the modulated Bi0.5 Na0.5 TiO3 (BNT)-based ceramics can demonstrate favorable energy storage properties with antiferroelectric-like properties, simultaneously, attaching superior temperature stability resulted from the high Curie temperature. Inspired by the above properties, a strategy is proposed to modulate antiferroelectric-like properties via introducing Ca0.7 La0.2 TiO3 (CLT) into Bi0.395 Na0.325 Sr0.245 TiO3 (BNST) ((1-x)BNST-xCLT, x = 0.10, 0.15, 0.20, 0.25). Combining both orthorhombic phase and defect dipole designs successfully achieve antiferroelectric-like properties in BNST-CLT ceramics. The results illustrate that 0.8BNST-0.2CLT presents superior recoverable energy storage density ≈8.3 J cm-3 with the ideal η ≈ 80% at 660 kV cm-1 . Structural characterizations demonstrate that there is the intermediate modulated phase with the coexistence of the antiferroelectric and ferroelectric phases. In addition, in situ temperature measurements prove that BNST-CLT ceramics exhibit favorable temperature stability over a wide temperature range. The present work illustrates that BNT-based ceramics with antiferroelectric-like properties can effectively enhance the energy storage performance, which provides novel perspectives for the subsequent development of advanced pulsed capacitors.

Synergistic Optimization of Energy Storage Density of PYN-Based Antiferroelectric Ceramics by Composition Design and Microstructure Engineering.

PbYb0.5 Nb0.5 O3 (PYN)-based ceramics, featured by their ultra-high phase-switching field and low sintering temperature (950 °C), are of great potential in exploiting dielectric ceramics with high energy storage density and low preparation cost. However, due to insufficient breakdown strength (BDS), their complete polarization-electric field (P-E) loops are difficult to be obtained. Here, to fully reveal their potential in energy storage, synergistic optimization strategy of composition design with Ba2+ substitution and microstructure engineering via hot-pressing (HP) are adopted in this work. With 2 mol% Ba2+ doping, a recoverable energy storage density (Wrec ) of 10.10 J cm-3 and a discharge energy density (Wdis ) of 8.51 J cm-3 can be obtained, supporting the superior current density (CD ) of 1391.97 A cm-2 and the outstanding power density (PD ) of 417.59 MW cm-2 . In situ characterization methods are utilized here to reveal the unique movement of the B-site ions of PYN-based ceramics under electric field, which is the key factor of the ultra-high phase-switching field. It is also confirmed that microstructure engineering can refine the grain of ceramics and improve BDS. This work strongly demonstrates the potential of PYN-based ceramics in energy storage field and plays a guiding role in the follow-up research.

Simultaneously achieving high performance of thermal stability and power consumption via doping yttrium in Sn15Sb85thin film.

The effects of yttrium dopants on the phase change behavior and microstructure of Sn15Sb85films have been systematically investigated. The yttrium-doped Sn15Sb85film has the higher phase transition temperature, ten year data retention ability and crystallization activation energy, which represent a great improvement in thermal stability and data retention. X-ray diffraction, transmission electron microscopy and x-ray photoelectron spectroscopy reveal that the amorphous Sn and Y components restrict the grain growth and decrease the grain size. Raman mode typically associated with Sb is altered when the substance crystallized. Atomic force microscopy results show that the surface morphology of the doped films becomes smoother. T-shaped phase change storage cells based on yttrium-doped Sn15Sb85films exhibit the lower power consumption. The results demonstrate that the crystallization characteristics of Sn15Sb85film can be tuned and optimized through the yttrium dopant for the excellent performances of phase change memory.

Delayed Polarization Saturation Induced Superior Energy Storage Capability of BiFeO3 -Based Ceramics Via Introduction of Non-Isovalent Ions.

Electrostatic capacitors are emerging as a highly promising technology for large-scale energy storage applications. However, it remains a significant challenge to improve their energy densities. Here, an effective strategy of introducing non-isovalent ions into the BiFeO3 -based (BFO) ceramic to improve energy storage capability via delaying polarization saturation is demonstrated. Accordingly, an ultra-high energy density of up to 7.4 J cm-3 and high efficiency ≈ 81% at 680 kV m-1 are realized, which is one of the best energy storage performances recorded for BFO-based ceramics. The outstanding comprehensive energy storage performance is attributed to inhibiting the polarization hysteresis resulting from generation ergodic relaxor zone and random field, and generating highly-delayed polarization saturation with continuously-increased polarization magnitudes with the electric field of supercritical evolution. The contributions demonstrate that delaying the polarization saturation is a consideration for designing the next generation of lead-free dielectric materials with ultra-high energy storage performance.

Superior Energy Storage Capability and Stability in Lead-Free Relaxors for Dielectric Capacitors Utilizing Nanoscale Polarization Heterogeneous Regions.

The development of high-performance lead-free dielectric ceramic capacitors is essential in the field of advanced electronics and electrical power systems. A huge challenge, however, is how to simultaneously realize large recoverable energy density (Wrec ), ultrahigh efficiency (η), and satisfactory temperature stability to effectuate next-generation high/pulsed power capacitors applications. Here, a strategy of utilizing nanoscale polarization heterogeneous regions is demonstrated for high-performance dielectric capacitors, showing comprehensive properties of large Wrec (≈6.39 J cm-3 ) and ultrahigh η (≈94.4%) at 700 kV cm-1 accompanied by excellent thermal endurance (20-160 °C), frequency stability (5-200 Hz), cycling reliability (1-105 cycles) at 500 kV cm-1 , and superior charging-discharging performance (discharge rate t0.9 ≈ 28.4 ns, power density PD ≈161.3 MW cm-3 ). The observations reveal that constructing the polarization heterogeneous regions in a linear dielectric to form novel relaxor ferroelectrics produces favorable microstructural characters, including extremely small polar nanoregions with high dynamics and multiphase coexistence and stable local structure symmetry, which enables large breakdown strength and ultralow polarization switching hysteresis, hence synergistically contributing to high-efficient capacitive energy storage. This study thus opens up a novel strategy to design lead-free dielectrics with comprehensive high-efficient energy storage performance for advanced pulsed power capacitors applications.

High Piezoelectricity in Eco-Friendly NaNbO3-Based Ferroelectric Relaxor Ceramics via Phase and Domain Engineering.

To meet the requirements of environmental friendliness, high-performance lead-free piezoelectric materials have become important materials for next-generation electronic devices. Here, lead-free and potassium-free NaNbO3 (NN)-based ceramics with high piezoelectric (d33 = 361 ± 10 pC/N) and dielectric (εr = 4500) properties were obtained by tolerant preparation techniques. The excellent piezoelectric and dielectric properties can be attributed to the relaxor morphotropic phase boundaries (R-MPB) and coexisting domain regions, which are beneficial in lowering the free energy and greatly improving the dielectric response and domain switching capability. Furthermore, the d33 of NaNbO3-10Ba(Ti0.7Sn0.3)O3-1.5NaSbO3 (NN-10BTS-1.5NS) ceramics can be maintained at 350 pC/N over the range of 25-80 °C with a change rate of less than 10%, exhibiting excellent temperature stability. Based on a series of in situ characterizations, the variations of the phase and domain structures of NN-based relaxor piezoelectric ceramics with temperature are clearly demonstrated. This work not only proposes new materials for sensors and actuators but also provides an excellent strategy for designing high-performance piezoelectric ceramics through phase and domain engineering.

Gradient-Structured Ceramics with High Energy Storage Performance and Excellent Stability.

Owing to the high power density, eco-friendly, and outstanding stability, the lead-free ceramics have attracted great interest in the fields of pulsed power systems. Nevertheless, the low energy storage density of such ceramics is undoubtedly a severe problem in practical applications. To overcome this limitation, the lead-free ceramics with gradient structures are designed and fabricated using the tape-casting method herein. By optimizing the composition and distribution of the gradient-structured ceramics, the energy storage density, and efficiency can be improved simultaneously. Under a moderate electric field of 320 kV cm-1 , the value of recoverable energy storage density (Wrec ) is higher than 4 J cm-3 , and the energy storage efficiency (η) is of ≥88% for 20-5-20 and 20-10-20. Furthermore, the gradient-structured ceramics of 20-10-0-10-20 and 20-15-0-15-20 possess high applied electric field, large maximum polarization, and small remnant polarization, which give rise to ultrahigh Wrec and η on the order of ≈6.5 J cm-3 and 89-90%, respectively. In addition, the energy storage density and efficiency also exhibit excellent stability over a broad range of frequencies, temperatures, and cycling numbers. This work provides an effective strategy for improving the energy storage capability of eco-friendly ceramics.

Polarity Modulation Induced High Electrostrain Performance with Near-Zero Hysteresis in a (Sr0.7Bi0.2□0.1)TiO3-Based System.

High-precision piezo actuators necessitate dielectrics with high electrostrain performance with low hysteresis. Polarity-modulated (Sr0.7Bi0.2□0.1)TiO3-based ceramics exhibit extraordinarily discrete multiphase coexistence regions: (i) the relaxor phase coexistence (RPC) region with local weakly polar tetragonal (T) and pseudocubic (Pc) short-range polar nanodomains and (ii) the ferroelectric phase coexistence (FPC) region with T long-range domains and Pc nanodomains. The RPC composition features a specially high and pure electrostrain performance with near-zero hysteresis (S ∼ 0.185%, Q33 ∼ 0.038 m4·C-2), which is double those of conventional Pb(Mg1/3Nb2/3)O3-based ceramics. Particular interest is paid to the RPC and FPC with multiscale characterization to unravel local structure-performance relationships. Guided by piezoelectric force microscopy, scanning transmission electron microscopy, and phase-field simulations, the RPC composition with multiphase low-angle weakly polar nanodomains shows local structural heterogeneity and contributes to a flat local free energy profile and thus to nanodomain switching and superior electrostrain performance, in contrast to the FPC composition with a macroscopic domain that shows stark hysteresis. This work provides a paradigm to design high-precision actuator materials with large electrostrain and ultralow hysteresis, extending our knowledge of multiphase coexistence species in ferroelectrics.

High Energy Storage Performance and Large Electrocaloric Response in Bi0.5Na0.5TiO3-Ba(Zr0.2Ti0.8)O3 Thin Films.

With regard to the global energy crisis and environmental pollution, ferroelectric thin films with unique polarization behavior have garnered considerable attention for energy storage and electrocaloric refrigeration. Herein, a series of (1 - x)Bi0.5Na0.5TiO3-xBa(Zr0.2Ti0.8)O3 (x = 0.3-0.9; (1 - x)BNT-xBZT) films were fabricated on Pt(111)/Ti/SiO2/Si substrates. Incorporating BZT can tune the polarization behavior and phase transition temperature of BNT. A high recoverable energy density ≈ 82 J cm-3 and optimized efficiency ≈ 81% were realized for the (1 - x)BNT-xBZT thin film with x = 0.7. The thin film exhibits excellent stability in energy storage performance, a wide working frequency range (0.5-20 kHz), a broad operating temperature window (20-200 °C), and reduplicative switching cycles (107 cycles). In addition, the 0.5BNT-0.5BZT film exhibits a desirable electrocaloric effect with a large adiabatic temperature change (ΔT ≈ -22.9 K) and isothermal entropy change (ΔS ≈ 33.4 J K-1 kg-1) near room temperature under a moderate applied electric field of 2319 kV cm-1. These remarkable performances signify that the (1 - x)BNT-xBZT system is a promising multifunctional electronic material for energy storage and solid-state cooling applications.

Boosting Energy Storage Performance of Lead-Free Ceramics via Layered Structure Optimization Strategy.

Owing to the current global scenario of environmental pollution and the energy crisis, the development of new dielectrics using lead-free ceramics for application in advanced electronic and energy storage systems is essential because of the high power density and excellent stability of such ceramics. Unfortunately, most of them have low breakdown strength and/or low maximum polarization, resulting in low energy density and efficiency. To overcome this limitation here, lead-free ceramics comprising a layered structure are designed and fabricated. By optimizing the distribution of the layered structure, a large maximum polarization and high applied electric field (>500 kV cm-1 ) can be achieved; these result in an ultrahigh recoverable energy storage density (≈7 J cm-3 ) and near ideal energy storage efficiency (≈95%). Furthermore, the energy storage performance without obvious deterioration over a broad range of operating frequencies (1-100 Hz), working temperatures (30-160 °C), and fatigue cycles (1-104 ). In addition, the prepared ceramics exhibit extremely high discharge energy density (4.52 J cm-3 ) and power density (405.50 MW cm-3 ). Here, the results demonstrate that the strategy of layered structure design and optimization is promising for enhancing the energy storage performance of lead-free ceramics.

Efficient Production of Solar Hydrogen Peroxide Using Piezoelectric Polarization and Photoinduced Charge Transfer of Nanopiezoelectrics Sensitized by Carbon Quantum Dots.

Piezoelectric semiconductors have emerged as redox catalysts, and challenges include effective conversion of mechanical energy to piezoelectric polarization and achieving high catalytic activity. The catalytic activity can be enhanced by simultaneous irradiation of ultrasound and light, but the existing piezoelectric semiconductors have trouble absorbing visible light. A piezoelectric catalyst is designed and tested for the generation of hydrogen peroxide (H2 O2 ). It is based on Nb-doped tetragonal BaTiO3 (BaTiO3 :Nb) and is sensitized by carbon quantum dots (CDs). The photosensitizer injects electrons into the conduction band of the semiconductor, while the piezoelectric polarization directed electrons to the semiconductor surface, allowing for a high-rate generation of H2 O2 . The piezoelectric polarization field restricts the recombination of photoinduced electron-hole pairs. A production rate of 1360 µmol gcatalyst -1  h-1  of H2 O2  is achieved under visible light and ultrasound co-irradiation. Individual piezo- and photocatalysis yielded lower production rates. Furthermore, the CDs enhance the piezocatalytic activity of the BaTiO3 :Nb. It is noted that moderating the piezoelectricity of BaTiO3 :Nb via microstructure modulation influences the piezophotocatalytic activity. This work shows a new methodology for synthesizing H2 O2  by using visible light and mechanical energy.

Tunable Domain Switching Features of Incommensurate Antiferroelectric Ceramics Realizing Excellent Energy Storage Properties.

An incommensurate modulated antiferroelectric phase is a key part of ideal candidate materials for the next generation of dielectric ceramics with excellent energy storage properties. However, there is less research carried out when considering its relatively low polarization response. Here, the incommensurate phase is modulated by stabilizing the antiferroelectric phase and the energy storage performance of the incommensurate phase under ultrahigh electric field is studied. The tape-casting method is applied to construct dense and thin ceramics. La3+ doping induces a room-temperature incommensurate antiferroelectric orthorhombic matrix. With little Cd2+ , the extremely superior energy storage performances arose as follows: when 0.03, the recoverable energy storage density reaches ≈19.3 J cm-3 , accompanying an ultrahigh energy storage efficiency of ≈91% (870 kV cm-1 ); also, a giant discharge energy density of ≈15.4 J cm-3 emerges during actual operation. In situ observations demonstrate that these superior energy storage properties originate from the phase transition from the incommensurate antiferroelectric orthorhombic phase to the induced rhombohedral relaxor ferroelectric one. The adjustable incommensurate period affects the depolarization response. The revealed phase-transition mechanism enriches the existing antiferroelectric-ferroelectric transition. Attention to the incommensurate phase can provide a reference for the selection of the next generation of high-performance antiferroelectric materials.