Large Energy Capacitive High-Entropy Lead-Free Ferroelectrics

Advanced lead-free energy storage ceramics play an indispensable role in next-generation pulse power capacitors market.Here,an ultrahigh energy storage density of~13.8 J cm^(-3)and a large efficiency of~82.4%are achieved in high-entropy lead-free relaxor ferroelectrics by increasing configuration entropy,named high-entropy strategy,realizing nearly ten times growth of energy storage density compared with low-entropy material.Evolution of energy storage performance and domain structure with increasing configuration entropy is systematically revealed for the first time.The achievement of excellent energy storage properties should be attributed to the enhanced random field,decreased nanodomain size,strong multiple local distortions,and improved breakdown field.Furthermore,the excellent frequency and fatigue stability as well as charge/discharge properties with superior thermal stability are also realized.The significantly enhanced comprehensive energy storage performance by increasing configuration entropy demonstrates that high entropy is an effective but convenient strategy to design new high-performance dielectrics,promoting the development of advanced capacitors.

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 leadfree,high-power ceramic capacitors.Ongoing efforts to develop leadfree dielectric ceramics with exceptional energystorage performance(ESP)have predominantly relied on multicomponent 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(Bi_(0.5)Na_(0.5))TiO_(3)(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 SrTiO_(3)(ST)into the BNT matrix is revealed to reduce the dielectric constant,while the addition of Bi(Mg_(2/3)Nb_(1/3))O_(3)(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(Bi_(0.5)Na_(0.4)K_(0.1))TiO_(3)–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℃ 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.

Relaxor antiferroelectric-relaxor ferroelectric crossover in NaNbO_(3)-based lead-free ceramics for high-efficiency large-capacitive energy storage

Relaxor ferroic dielectrics have garnered increasing attention in the past decade as promising materials for energy storage.Among them,relaxor antiferroelectrics(AFEs)and relaxor ferroelectrics(FEs)have shown great promise in term of high energy storage density and efficiency,respectively.In this study,a unique phase transition from relaxor AFE to relaxor FE was achieved for the first time by introducing strong-ferroelectricity BaTiO_(3)into NaNbO_(3)-BiFeO_(3)system,leading to an evolution from AFE R hierarchical nanodomains to FE polar nanoregions.A novel medium state,consisting of relaxor AFE and relaxor FE,was identified in the crossover of 0.88NaNbO_(3)–0.07BiFeO_(3)–0.05BaTiO_(3)ceramic,exhibiting a distinctive core-shell grain structure due to the composition segregation.By harnessing the advantages of high energy storage density from relaxor AFE and large efficiency from relaxor FE,the ceramic showcased excellent overall energy storage properties.It achieved a substantial recoverable energy storage density W_(rec)~13.1 J/cm^(3)and an ultrahigh efficiencyη~88.9%.These remarkable values shattered the trade-off relationship typically observed in most dielectric capacitors between W_(rec)andη.The findings of this study provide valuable insights for the design of ceramic capacitors with enhanced performance,specifically targeting the development of next generation pulse power devices.

Lead-free BiFeO_(3)-BaTiO_(3) based high-Tc ferroelectric ceramics:Antiferroelectric chemical modification leading to high energy storage performance

Dielectric capacitors have been widely used in pulsed power devices owing to their ultrahigh power density,fast charge/discharge speed,and excellent stability.However,developing lead-free dielectric materials with a combination of high recoverable energy storage density and efficiency remains a challenge.Herein,a high energy storage density of 7.04 J/cm^(3) as well as a high efficiency of 80.5%is realized in the antiferroelectric Ag(Nb_(0.85)Ta_(0.15))O_(3)-modified BiFeO3-BaTiO3 ferroelectric ceramic.This achievement is mainly attributed to the combined effect of a high saturation polarization(Pmax),increased breakdown field(Eb),and reduction of the remnant polarization(Pr).The modification of pseudotetragonal BiFeO3 by Ag(Nb_(0.85)Ta_(0.15))O_(3) leads to a high Pmax,and the enhanced relaxor behavior gives rise to a small Pr.The promoted microstructure(such as a dense structure,fine grains,and compact grain boundaries)after modification results in a high breakdown strength.Furthermore,both the recoverable energy density and efficiency exhibit high stability over a broad range of operating frequencies(1–50 Hz)and working temperatures(25–120℃).These results suggest that the(0.67–x)BiFeO_(3)-0.33BaTiO_(3)-xAg(Nb_(0.85)Ta_(0.15))O_(3) ceramics can be highly competitive as a lead-free relaxor for energy storage applications.

Excellent energy storage performance in Bi_(0.5)Na_(0.5)TiO_(3)-based lead-free high-entropy relaxor ferroelectrics via B-site modification

Next-generation advanced high/pulsed power capacitors urgently require dielectric materials with outstanding energy storage performance.Bi_(0.5)Na_(0.5)TiO_(3)-based lead-free materials exhibit high polarization,but the high remanent polarization and large polarization hysteresis limit their applications in dielectric capacitors.Herein,high-entropy perovskite relaxor ferroelectrics(Na_(0.2)Bi_(0.2)Ba_(0.2)Sr_(0.2)Ca_(0.2))(Ti1-x%Zrx%)O_(3)are designed by adding multiple ions in the A-site and replacing the B-site Ti^(4+)with a certain amount of Zr^(4+).The newly designed system showed high relaxor feature and slim polarization-electric(P-E)loops.Especially,improved relaxor feature and obviously delayed polarization saturation were found with the increasing of Zr^(4+).Of particular importance is that both high recoverable energy storage density of 6.6 J/cm^(3) and energy efficiency of 93.5%were achieved under 550 kV/cm for the ceramics of x=6,accompanying with excellent frequency stability,appreciable thermal stability,and prosperous discharge property.This work not only provides potential dielectric materials for energy storage applications,but also offers an effective strategy to obtain dielectric ceramics with ultrahigh comprehensive energy storage performance to meet the demanding requirements of advanced energy storage applications.

Influences of Ho Doping on Structure,Ferroelectric,Energy Storage and Optical Properties of KNN-SYbN Transparent Ceramics

Ho doping 0.825K_(0.5)Na_(0.5)NbO_(3)-0.175Sr(Yb_(0.5)Nb_(0.5))_(O3)(KNN-SYbN-x%Ho)transparent ceramics were prepared by solid-state sintering method.The structure,ferroelectric,energy storage,and optical properties of KNN-SYbN-x%Ho were explored.With the addition of Ho,under the excitation of a 980 nm laser,the ceramics exhibit up-conversion luminescence properties with wavelengths of 550 nm and 670 nm,however,the ceramics change from pseudo-cubic phase to triphase-orthorhombic phase and the light transmittance decreases.The addition of Ho significantly enhances the ferroelectric properties and the energy storage performance of KNN-SYbN-x%Ho ceramics.When x=0.15,the residual polarization P_(r)=9.11μC/cm^(2),while x=0.20,the maximum energy storage density W_(rec) reaches 0.26 J/cm^(3),and the energy storage efficiencyηreaches 87.1%.

Improved energy storage performance of bismuth sodium titanate-based lead-free relaxor ferroelectric ceramics via Bi-containing complex ions doping

Lead-free dielectric ceramics can be used to make quick charge-discharge capacitor devices due to their high power density.Their use in advanced electronic systems,however,has been hampered by their poor energy storage performance(ESP),which includes low energy storage efficiency and recoverable energy storage density(Wrec).In this work,we adopted a combinatorial optimization strategy to improve the ESP in(Bi_(0.5)Na_(0.5))TiO_(3)(BNT)-based relaxor ferroelectric ceramics.To begin,the Bi-containing complex ions Bi(Mg_(2/3)Nb_(1/3))O_(3)(BMN)were introduced into a BNT-based matrix in order to improve the diffuse phase transition,increase Bi-O bond coupling,avoid macro domain development,and limit polarization response hysteresis.Second,the viscous polymer process was employed to reduce sample thickness and porosity,resulting in an apparent increase in breakdown strength in(1-x)[0.7(Bi_(1/2)Na_(1/2))TiO_(3)]-0.3SrTiO_(3)-xBi(Mg_(2/3)Nb_(1/3))O_(3)(BS-xBMN)ceramics.Finally,in x=0.20 composition,an amazing Wrecof 5.62 J·cm^(-3)and an ultra-high efficiency of 91.4%were simultaneously achieved at a relatively low field of 330 kV·cm^(-1),together with remarkable temperature stability in the temperature range of 30-140℃(3.5 J·cm^(-3)±5%variation).This research presents a new lead-free dielectric material with superior ESP for use in pulsed power capacitors.

Stress-induced tailoring of energy storage properties in lead-free Ba_(0.85)Ca_(0.15)Zr_(0.1)Ti_(0.9)O_(3)ferroelectric bulk ceramics

In this study,the stress-modulated energy storage properties of lead-free polycrystalline Ba_(0.85)Ca_(0.15)Zr_(0.1)Ti_(0.9)O_(3)was investigated as a function of temperature from 25℃to 55℃.The externally applied uniaxial compressive stress of-160 MPa increased the recoverable energy storage density by 226%to a maximum value of 274 mJ/cm^(3),in addition to enhancing the energy storage efficiency by approximately 10%to a value of 88.2%.The macroscopic mechanical constitutive behavior is presented as well as the stress-dependent dielectric and ferroelectric properties and the Rayleigh behavior in order to elucidate the effect of stress on the energy storage properties.Importantly,the stress-induced tailoring of energy storage performance can be utilized for other nonlinear dielectric ceramics to tune their extrinsic polarization mechanisms to significantly enhance the recoverable energy density and reduce the hysteretic losses.

High energy storage properties in Ca_(0.7)La_(0.2)TiO_(3)-modified NaNbO_(3)-based lead-free antiferroelectric ceramics

In this work,(1−x)(0.92NaNbO_(3)-0.08BaTiO_(3))-xCa_(0.7)La_(0.2)TiO_(3)(NNBT-xCLT)ceramics were successfully designed and pre­pared by the solid-state reaction method.Investigations on the structure,dielectric,and energy storage properties were performed.The NNBT-0.25CLT ceramic with orthorhombic phase at room temperature was found to exhibit extremely small grain size and compacted microstructure.A large Wrec of 3.1 J/cm^(3) and a highηof 91.5%under the electric field of 360 kV/cm were achieved simultaneously in the sample.In addition,the energy storage performance of the sample exhibits thermal stability over the tem­perature range of 25-140°C and the frequency range of 5-500 Hz.The charge and discharge tests reveal that the ceramic shows a large current density CD of 965 A/cm2 and power density PD of 154 MW/cm^(3).This work demonstrates that the NNBT-0.25CLT ceramic is a prospective energy storage material for potential application in the field of pulsed power devices.

Enhancing energy storage efficiency in lead-free dielectric ceramics through relaxor and lattice strain engineering

Dielectric capacitors with high power density and fast charge-discharge speed play an essential role in the development of pulsed power systems.The increased demands for miniaturization and practicality of pulsed power equipment also necessitate the development of dielectric materials that possess high energy density while maintaining ultrahigh efficiency(η).In particular,ultrahigh efficiency signifies minimal energy loss,which is essential for practical applications but challenging to effectively mitigate.Here,we demonstrate a strategy of incorporating heterovalent elements into Ba(Zr_(0.1)Ti_(0.9))O_(3),which contributes to achieving relaxor ferroelectric ceramics and reducing lattice strain,thereby improving the comprehensive energy storage performance.Finally,optimal energy storage performance is attained in 0.85Ba(Zr_(0.1)Ti_(0.9))O_(3)-0.15Bi(Zn_(2/3)Ta_(1/3))O_(3)(BZT-0.15BiZnTa),with an ultrahighηof 97.37%at 440 kV/cm(an advanced level in the lead-free ceramics)and an excellent recoverable energy storage density(Wrec)of 3.74 J/cm^(3).Notably,the BZT-0.15BiZnTa ceramics also exhibit exceptional temperature stability,maintaining fluctuations in Wrec within∼10%andηconsistently exceeding 90% across the wide temperature range of−55℃ to 160℃,and under a high electric field of 250 kV/cm.All these features demonstrate that the relaxor and lattice strain engineering strategies have been successful in achieving high-performance lead-free ceramics,paving the way for designing high-efficiency dielectric capacitors with a wide temperature range.

A novel lead-free relaxor with endotaxial nanostructures for capacitive energy storage

Dielectric capacitors with a fast charging/discharging rate,high power density,and long-term stability are essential components in modern electrical devices.However,miniaturizing and integrating capacitors face a persistent challenge in improving their energy density(W_(rec))to satisfy the specifications of advanced electronic systems and applications.In this work,leveraging phase-field simulations,we judiciously designed a novel lead-free relaxor ferroelectric material for enhanced energy storage performance,featuring flexible distributed weakly polar endotaxial nanostructures(ENs)embedded within a strongly polar fluctuation matrix.The matrix contributes to substantially enhanced polarization under an external electric field,and the randomly dispersed ENs effectively optimize breakdown phase proportion and provide a strong restoring force,which are advantageous in bolstering breakdown strength and minimizing hysteresis.Remarkably,this relaxor ferroelectric system incorporating ENs achieves an exceptionally high W_(rec)value of 10.3 J/cm^(3),accompanied by a large energy storage efficiency(η)of 85.4%.This work introduces a promising avenue for designing new relaxor materials capable of capacitive energy storage with exceptional performance characteristics.

Design strategies of high-performance lead-free electroceramics for energy storage applications

A greater number of compact and reliable electrostatic capacitors are in demand due to the Internet of Things boom and rapidly growing complex and integrated electronic systems,continuously promoting the development of high-energy-density ceramic-based capacitors.Although significant successes have been achieved in obtaining high energy densities in lead-based ferroelectric ceramics,the utilization of lead-containing ceramies has been restricted due to environmental and health hazards of lead.Lead-free ferroelectric ceramics have garnered tremendous attention and are expected to replace lead-based ceramics in the near future.However,the energy density of lead-free ceramics is still lagging behind that of lead-containing cou.nterparts,severely limiting their applications.Significant efforts have been made to enhance the energy storage performance of lead-free ceramics using multi-scale design strategies,and exciting progress has been achieved in the past decade.This review briefly discusses the energy storage mechanism and fundamental characteristics of a dielectric capacitor,summarizes and compares the state-of-the-art design strategies for high-energy-density lead-free ceramics,and highlights several critical issues and requirements for industrial production.The prospects and challenges of lead-free ceramics for energy storage applications are also discussed.

Energy storage optimization of ferroelectric ceramics during phase-transition process of amorphous/nanocrystalline and polycrystalline by using a phaseffeld model for dielectric breakdown

Ferroelectric ceramics have the potential to be widely applied in the modern industry and military power systems due to their ultrafast charging/discharging speed and high energy density.Considering the structural design and electrical properties of ferroelectric capacitor,it is still a challenge to ffnd out the optimal energy storage of ferroelectric ceramics during the phase-transition process of amorphous/nanocrystalline and polycrystalline.In this work,a ffnite element model suitable for the multiphase ceramic system is constructed based on the phase ffeld breakdown theory.The nonlinear coupling relationship of multiple physical ffelds between multiphase ceramics was taken into account in this model.The basic structures of multiphase ceramics are generated by using the Voronoi diagram construction method.The speciffed structure of multiphase ceramics in the phase-transition process of amorphous/nanocrystalline and polycrystalline was further obtained through the grain boundary diffusion equation.The simulation results show that the multiphase ceramics have an optimal energy storage in the process of amorphous polycrystalline transformation,and the energy storage density reaches the maximum when the crystallinity is 13.96%and the volume fraction of grain is 2.08%.It provides a research plan and idea for revealing the correlation between microstructure and breakdown characteristics of multiphase ceramics.This simulation model realizes the nonlinear coupling of the multiphase ceramic mesoscopic structure and the phase ffeld breakdown.It provides a reference scheme for the structural design and performance optimization of ferroelectric ceramics.

Combinatorial optimization of perovskite-based ferroelectric ceramics for energy storage applications

With the increasing impacts of climate change and resource depletion,dielectric capacitors,with their exceptional stability,fast charging and discharging rates,and ability to operate under more extreme conditions,are emerging as promising high-demand candidates for high-performance energy storage devices,distinguishing them from traditional electrochemical capacitors and batteries.However,due to the shortcomings of various dielectric ceramics(e.g.,paraelectrics(PEs),ferroelectrics(FEs),and antiferroelectrics(AFEs)),their low polarizability,low breakdown strength(BDS),and large hysteresis loss limit their standalone use in the advancement of energy storage ceramics.Therefore,synthesizing novel perovskite-based materials that exhibit high energy density,high energy efficiency,and low loss is crucial for achieving superior energy storage performance.In this review,we outline the recent development of perovskitebased ferroelectric energy storage ceramics from the perspective of combinatorial optimization for tailoring ferroelectric hysteresis loops and comprehensively discuss the properties arising from the different combinations of components.We also provide future guidelines in this realm.Therefore,the combinatorial optimization strategy in this review will open up a practical route toward the application of new high-performance ferroelectric energy storage devices.

Enhanced energy storage properties and good stability of novel(1-x)Na_(0.5)Bi_(0.5)TiO_(3)-xCa(Mg_(1/3)Nb_(2/3))O_(3) relaxor ferroelectric ceramics prepared by chemical modification

The increase in energy consumption and its collateral damage on the environment has encouraged the development of environment-friendly ceramic materials with good energy storage properties.In this work,(1-x)Na_(0.5)Bi_(0.5)TiO_(3)-xCa(Mg_(1/3)Nb_(2/3))O_(3) ceramics were synthesized by the solid-state reaction method.The 0.88Na_(0.5)Bi_(0.5)TiO_(3)-0.12Ca(Mg_(1/3)Nb_(2/3))O_(3) ceramic exhibited a high recoverable energy storage density of 8.1 J/cm3 and energy storage efficiency of 82.4% at 550 kV/cm.The introduction of Ca(Mg_(1/3)Nb_(2/3))O_(3) reduced the grain size and increased the band gap,thereby enhancing the breakdown field strength of the ceramic materials.The method also resulted in good temperature stability(20–140℃),frequency stability(1–200 Hz),and fatigue stability over 106 cycles.In addition,an ultrahigh power density of 187 MW/cm^(3) and a fast charge-discharge rate(t0.9=57.2 ns)can be obtained simultaneously.Finite element method analysis revealed that the decrease of grain size was beneficial to the increase of breakdown field strength.Therefore,the 0.88Na_(0.5)Bi_(0.5)TiO_(3)-0.12Ca(Mg_(1/3)Nb_(2/3))O_(3) ceramics resulted in high energy storage properties with good stability and were promising environment-friendly materials for advanced pulsed power systems applications.

Polymer-/Ceramic-based Dielectric Composites for Energy Storage and Conversion

Dielectric composites boost the family of energy storage and conversion materials as they can take full advantage of both the matrix and filler.This review aims at summarizing the recent progress in developing highperformance polymer-and ceramic-based dielectric composites,and emphases are placed on capacitive energy storage and harvesting,solid-state cooling,temperature stability,electromechanical energy interconversion,and high-power applications.Emerging fabrication techniques of dielectric composites such as 3D printing,electrospinning,and cold sintering are addressed,following by highlighted challenges and future research opportunities.The advantages and limitations of the typical theoretical calculation methods,such as finite-element,phase-field model,and machine learning methods,for designing high-performance dielectric composites are discussed.This review is concluded by providing a brief perspective on the future development of composite dielectrics toward energy and electronic devices.

High energy-storage properties of Bi_(0.5)Na_(0.5)TiO_3-BaTiO_3-SrTi_(0.875)Nb_(0.1)O_3 lead-free relaxor ferroelectrics

New lead-free ferroelectric(0.94-x)BioNaTiO-0.06 BaTiOSrTiNbO(BNBT-STN,x = 0 and 0.2)are synthesized by using a solid state reaction process. In this work, an obvious evolution of dielectric relaxation behavior and slim P-E hysteresis loops with high Pmax and low Pr is observed for BNBT-0.2 STN,indicating the dominant of ergodic relaxor phase with dynamic polar nano-regions(PNRs). A relatively large recoverable energy density(Wrec = 1.17 J/cm~3) with high energy efficiency(η= 91%) is obtained. Furthermore, it shows small variation(9%) in the temperature range of 30-150 ℃ and fatigue-free behavior,which can be attributed to the absence of ferroelectric domain in the relaxor phase. The achievement of these characteristics provides that tailoring by B-site vacancies is a potential route when designing a new energy-storage system for BNT-based relaxor ferroelectric materials.

High energy storage density and power density achieved simultaneously in NaNbO_(3)-based lead-free ceramics via antiferroelectricity enhancement

High-performance lead-free dielectric ceramics with simultaneously high energy storage density and power density are in high demanded for pulse power systems.To realize excellent energy-storage characteristics,a strategy to enhance antiferroelectricity and construct a local random field simultaneously was proposed in this study.Based on the above strategy,a series of(1-x)NaNbO_(3)-xBi(Ni_(1/2)Sn_(1/2))O3[xBNS,x=0.05,0.10,0.15,0.20,and 0.22]solid solutions were designed and fabricated.An ultrahigh energy storage density(Utotal)of 7.35 J/cm^(3),and recoverable energy density(Urec)of 5.00 J/cm^(3) were achieved in the 0.10BNS ceramics.In addition,an adequate stability of energy storage properties at a range of temperatures(20e140℃),frequencies(1e100 Hz),and fatigue test durations(1e1-10^(4) cycles)were realized in 0.10BNS ceramics.0.10BNS ceramics displayed a high current density of 1005 A/cm2,an ultrahigh power density of 100.5 MW/cm^(3,)and an ultrashort discharge time of 46.5 ns?This remarkable performance not only justified our strategy but also confirmed 0.10BNS ceramics as a promising candidate for energy storage.

Novel lead-free NaNbO_(3) -based relaxor antiferroelectric ceramics with ultrahigh energy storage density and high efficiency

The development of environmentally friendly ceramics for electrostatic energy storage has drawn growing interest due to the wide application in high power and/or pulsed power electronic systems.However,it is difficult to simultaneously achieve ultrahigh recoverable energy storage density(W rec>8 J/cm^(3))and high efficiency(η>80%),which restricts their application in the miniaturized,light weight and easy integrated electronic devices.Herein,the novel NaNbO_(3)-(Bi_(0.8)Sr_(0.2))(Fe_(0.9) Nb_(0.1))O_(3) relaxor antiferro-electric ceramics,which integrates the merits of antiferroelectrics and relaxors,are demonstrated to exhibit stabilized antiferroelectric phase and enhanced dielectric relaxor behavior.Of particular impor-tance is that the 0.88NN-0.12BSFN ceramic achieves giant electric breakdown strength E_(b)=98.3 kV/mm,ultrahigh W _(rec)=16.5 J/cm^(3) and high h=83.3%,as well as excellent frequency,cycling and thermal reliability simultaneously.The comprehensive energy storage performance of NN-BSFN not only out-performs state-of-the-art dielectric ceramics by comparison,but also displays outstanding potential for next-generation energy storage capacitors.

Superior energy storage efficiency through tailoring relaxor behavior and band energy gap in KNN-based ferroelectric ceramic capacitors

With the increasing demand of high-power and pulsed power electronic devices,environmental-friendly potassium sodium niobate((Na_(0.5)K_(0.5))NbO_(3),KNN)ceramic-based capacitors have attracted much attention in recent years owning to the boosted energy storage density(W_(rec)).Nevertheless,the dielectric loss also increases as the external electric field increases,which will generate much dissipated energy and raise the temperature of ceramic capacitors.Thus,an effective strategy is proposed to enhance the energy storage efficiency(η)via tailoring relaxor behavior and bad gap energy in the ferroelectric 0.9(Na_(0.5)K_(0.5))-NbO_(3)-0.1Bi(Zn_(2/3)(Nb_(x)Ta_(1−x))1/3)O_(3) ceramics.On the one hand,the more diverse ions in the B-sites owing to introducing the Ta could further disturb the long-range ferroelectric polar order to form the short−range polar nanoregions(PNRs),resulting in the highη.On the other hand,the introduction of Ta ions could boost the intrinsic band energy gap and thus improve the Eb.As a result,high Wrec of 3.29 J/cm^(3) and ultrahighηof 90.1%at the high external electric field of 310 kV/cm are achieved in x=0.5 sample.These results reveal that the KNN-based ceramics are promising lead-free candidate for high-power electronic devices.