Ultrahigh energy storage performance in Pb0.94La0.04Zr0.99Ti0.01O3 ceramics via introducing pyrochlore phase Y2Zr2O7

Ultrahigh energy storage performance in Pb0.94La0.04Zr0.99Ti0.01O3 ceramics via introducing pyrochlore phase Y2Zr2O7 | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Research Article Ultrahigh energy storage performance in Pb 0.94 La 0.04 Zr 0.99 Ti 0.01 O 3 ceramics via introducing pyrochlore phase Y 2 Zr 2 O 7 Lei Cao, Bowen Huang, Tianci Yang, Chenglong Jiang, Ye Zhao, Pei Han, and 5 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-9095268/v1 This work is licensed under a CC BY 4.0 License Status: Posted Version 1 posted You are reading this latest preprint version Abstract Antiferroelectric (AFE) ceramics hold great promise for high energy density capacitors, though their energy storage properties (ESPs) are fundamentally limited by a relatively low breakdown electric field ( E b ). Hence, the dual-phase composite ceramics were designed by incorporating a pyrochlore phase into the perovskite matrix to enhance ESPs. Composite ceramics of Y 2 Zr 2 O 7 modified Pb 0.94 La 0.04 Zr 0.99 Ti 0.01 O 3 - x wt% Y 2 O 3 were fabricated and investigated. The introduction of Y 2 Zr 2 O 7 serves to reduce the overall dielectric permittivity ( ε r ) and enhance insulation, which collectively raise the E b from 420 kV/cm to 850 kV/cm. A maximum recoverable energy density ( W rec ) of 14.5 J/cm 3 with an energy efficiency ( η ) of 85.7% are achieved in the ceramic with x = 4 under 570 kV/cm. In addition, a current density ( C D ) as high as 2369.4 A/cm 2 , a power density ( P D ) of 462 MW/cm 3 , and an ultrafast discharge rate of 22.6 ns are achieved. This work establishes the construction of dual-phase composites as a viable and novel approach to improving ESPs in PbZrO 3 (PZ) -based ceramic systems. Antiferroelectric Energy storage performances Dual-phase composite ceramics Y2O3 Breakdown strength Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 1. Introduction Ceramic capacitors exhibit broad application prospects in electric vehicles, pulse power systems, and other fields due to their excellent charge-discharge rates and high power density ( P D )[ 1 – 3 ]. However, the relatively low energy storage density remains a key bottleneck limiting their miniaturization and integration. Therefore, improving energy storage properties (ESPs) is of significant scientific importance and practical value. In general, the total energy storage density ( W tot ), recoverable energy storage density ( W rec ) and energy storage efficiency ( η ) of dielectric ceramic capacitors can be calculated using the following formulas[ 4 ]: $$\:\begin{array}{c}{\text{W}}_{\text{tot}}\text{}\text{=}\text{}{\int\:}_{\text{0}}^{{\text{P}}_{\text{max}}}\text{EdP}\#\left(1\right)\end{array}$$ $$\:\begin{array}{c}{\text{W}}_{\text{rec}}\text{}\text{=}\text{}{\int\:}_{{\text{P}}_{\text{r}}}^{{\text{P}}_{\text{max}}}\text{EdP}\#\left(2\right)\end{array}$$ $$\:\begin{array}{c}\text{ɳ}\text{=}\text{}\frac{{\text{W}}_{\text{rec}}}{{\text{W}}_{\text{tot}}}\text{×}\text{100}\text{%}\#\left(3\right)\end{array}$$ where E , P r , and P max denote as the applied electric field, remanent polarization, and maximum polarization, respectively. The formulas reveal that achieving a high W rec necessitates concurrently high P max , low P r and high breakdown field ( E b ). Among these, pursuing E b optimization emerges as a particularly effective strategy, as the improvement from polarization enhancement alone is intrinsically constrained[ 5 ]. PbZrO 3 (PZ) -based antiferroelectric (AFE) ceramics are considered one of the most promising energy storage dielectric ceramics for achieving high W rec due to their unique double hysteresis loops and high P max and near-zero P r [ 6 ]. The ESPs of PZ-based AFE materials are primarily constrained by their low E b . Consequently, rare-earth ion doping has been widely adopted as a feasible strategy to enhance E b and thereby improve ESPs[ 7 ]. For example, Yang et al. demonstrated that Nd 3+ doping stabilized the AFE phase in a Pb 0.98 Sr 0.02 Zr 0.75 Sn 0.25 O 3 (PSrZS) ceramics, increasing its E b from 350 kV/cm to 540 kV/cm and resulting in a high W rec of 14.21 J/cm 3 with η of 87.35%[ 8 ]. In addition to ion doping, constructing dual-phase composite ceramics is also an effective strategy to improve the breakdown characteristics of dielectric ceramics[ 9 ]. For example, Pan et al. introduced the pyrochlore Sm 2 Sn 2 O 7 into a Bi 0.5 Na 0.5 TiO 3 (BNT) -based perovskite matrix, raising the E b from 220 to 700 kV/cm and achieving a W rec of 9.91 J/cm 3 with η of 87.01%[ 10 ]. Such enhanced ESPs are attributed to the existence of pyrochlore phase in perovskite matrix, which possesses a low dielectric constant ( ε r ), wide bandgap ( E g ), low dielectric loss (tan δ ), and high stability[ 11 – 13 ]. Therefore, constructing a composite structure by introducing a pyrochlore phase (Y 2 Zr 2 O 7 ) into perovskite dielectric ceramics is a promising strategy to significantly enhance ESPs, offering broad application prospects. Y 2 Zr 2 O 7 is a pyrochlore phase transparent ceramic with a low ε r (~ 27), wide E g (~ 4.5 eV), low tan δ (~ 0.001), and high thermal resistance (1.2 ~ 1.3 W/(m·k)). While currently utilized mainly in phosphors and photochromism applications, distinctive dielectric properties also render it a promising candidate for energy storage applications[ 14 – 18 ]. Previous studies indicate that doping Y 3+ into the A-site can induce local chemical disorder, disrupt the original long-range ferroelectric order of the PZ-based ceramics, and promote a transition to a diffuse relaxor state. Simultaneously, it helps to reduce oxygen vacancy concentration, refine grain size, and enhance E b [ 19 ]. In this work, a series of Pb 0.94 La 0.04 Zr 0.99 Ti 0.01 O 3 (PLZT) - x wt% Y 2 O 3 ceramics were designed by introducing x wt% Y 2 O 3 at the initial mixing stage. This non-equivalent doping strategy promotes the directional formation of a secondary phase within the PLZT matrix. Consequently, it enhances the stability of the AFE state and simultaneously improves the E b , leading to excellent overall ESPs. This work offers a promising composite ceramic candidate for pulsed power systems. 2. Experimental Section Antiferroelectric ceramics with the composition of Pb 0.94 La 0.04 Zr 0.99 Ti 0.01 O 3 - x wt%Y 2 O 3 with x = 0, 2, 4, 6, and 8 were prepared by a tape-casting. These samples are accordingly designated as Y0, Y2, Y4, Y6 and Y8. The starting materials are lead tetroxide (Pb 3 O 4 , 95.0%), yttrium oxide (Y 2 O 3 , 99.9%), zirconium dioxide (ZrO 2 , 99.0%), titanium dioxide (TiO 2 , 99.5%), lanthanum oxide (La 2 O 3 , 99.9%). PLZT (Pb 0.94 La 0.04 Zr 0.99 Ti 0.01 O 3 ) were weighed according to the stoichiometric ratio, but yttrium oxide is doped in proportion to the mass of the corresponding powder. All raw materials ball milled in alcohol for 24 h. The mixture was calcined at 900 o C for 2 h, followed by grinding and a second 24 h ball-milling. After drying and sieving, the powder was shaped via tape-casting, subsequently air-dried, and densified through sequential hot pressing and cold isostatic pressing. Organic components were removed at 600 o C for 5 h. The samples were sintered at 1160 o C for 3 h, polished to a thickness of ~ 70 µm, and coated with 1 mm-diameter gold electrodes via ion suppering for electrical properties. The crystal structure was characterized using X-ray diffraction (XRD; Bruker D8 Advance) with Cu K α radiation. The obtained diffraction patterns were refined using the Rietveld method in GSAS-II software. Microstructure analysis was conducted using a scanning electron microscope (SEM; Thermo Fisher MIRA3) operated in backscattered electron (BSE) mode. The impedance spectrum was measured using an impedance analyzer (Agilent E4990A). The polarization-electric field ( P - E ) hysteresis loops and current-electric field ( I - E ) curve loops were measured using a ferroelectric testing system integrated with a temperature-controlled probe station (Radiant Technologies) at 10 Hz. The charge-discharge performance was evaluated using a dedicated pulse power platform (Gogo Instruments CFD137005) connected to a DC power supply (ENTAI ET2671A). 3. Results and Discussion Figure 2 (a) presents the XRD pattern of the PLZT- x wt% Y 2 O 3 ceramic. The main crystalline phase corresponds to a typical perovskite structure (PDF# 97-016-6843) with an orthorhombic symmetry. With increasing Y 2 O 3 content, diffraction peaks corresponding to the cubic pyrochlore phase Y 2 Zr 2 O 7 (PDF# 97-015-3818) gradually emerge, and their intensities progressively increase. The results indicate that excessive Y 2 O 3 doping exceeds the solid solubility limit in the PLZT matrix, leading to the precipitation of the secondary phase[ 20 ]. To quantify the relative content of the perovskite and pyrochlore phases, the Rietveld refinement was conducted. As shown in Fig. 2 (b), the Rietveld refinement results of Y0 and Y4 ceramics indicate that all samples exhibit a typical perovskite structure, and the content of pyrochlore phase monotonically increases with the increase of Y 3+ content. The refinement was carried out simultaneously based on two spatial group models: orthorhombic phase Pba2 and cubic phase Fd-3m. All the samples exhibit low R -factors ( R wp < 10%), and unit cell parameters for Y4 ceramics are provided in Fig. S1 . These results confirm the validity of the structural models and the reliability of the refinement, with the calculated patterns showing excellent agreement with the experimental data[ 21 ]. The XRD Rietveld refinement patterns for ceramics Y2, Y6 and Y8 are provided in Fig. S2. It can be seen that the formation of the Y 2 Zr 2 O 7 pyrochlore phase increases the cubic phase fraction to 8.8% in Y2 sample. With further increase in Y 2 O 3 addition, it reaches 48% in Y4 and eventually rises nonlinearly to 60.4% in Y8 (Fig. 2 (c)). This evolution is attributed to the limited solubility of Y 2 O 3 in the PLZT lattice. This limited solubility disrupts the long-range ferroelectric order, thereby enhancing the relaxor behavior of the materials [ 22 ]. To further elucidate the influence of Y 2 O 3 on the structural characteristics, room-temperature Raman spectra were collected ( Fig. S3 ). A detailed Gaussian-Lorentzian fitting analysis was conducted on the Raman spectra of the Y0 and Y4 samples, as shown in Fig. 2 (d). The spectral features are systematically divided into three distinct regions: A-site ion vibrations (50 ~ 150 cm − 1 ), B-O bond vibrations (150 ~ 450 cm − 1 ), and BO 6 octahedral vibrations (450 ~ 800 cm − 1 ). The Y4 sample exhibits significant spectral alterations in the low-frequency region (< 150 cm − 1 ) compared to Y0, resulting from the perturbation of A-site vibrational modes by Y 3+ doping. Concurrently, the Raman peak near 220 cm − 1 shifts in position and exhibits a reduced full width at half maximum (FWHM), indicating enhanced lattice distortion [ 23 ]. Furthermore, in the region of 450 ~ 800 cm − 1 , the absence of a characteristic J-fitting peak in Y4 sample suggests that the precipitation of the secondary phase enhances the structural stability of the BO 6 octahedra. As shown in Fig. 2 (e) and (f), both Y0 and Y4 ceramics exhibit well-defined grain with sharp boundaries and a dense microstructure, indicating the suitability of the sintering temperature. The BSE images (Fig. 2 (f)) reveal the stable coexistence of pyrochlore phase Y 2 Zr 2 O 7 and perovskite phase PLZT in the Y4 ceramic, which has been consistently reproduced in repeated experiments. This indicates that the significant enhancement in E b is not due to grain size effects[ 22 ]. To identify the composition of the second phase, energy-dispersive X-ray spectroscopy (EDS) was conducted on all samples, as shown in Fig. S4 . The results demonstrate a distinct co-enrichment of Y 3+ and Zr 4+ ions in Y4 samples, confirming the formation of the Y 2 Zr 2 O 7 secondary phase[ 23 ]. The breakdown reliability was evaluated using Weibull distribution analysis, as shown in Fig. 3 (a). All the PLZT- x wt% Y 2 O 3 ceramics exhibit a Weibull modulus ( β ) higher than 10, indicating excellent consistency and high reliability of the E b [ 24 ]. The E b of Y0, Y2, Y4, Y6, and Y8 ceramics are 440 kV/cm, 490 kV/cm, 570 kV/cm, 720 kV/cm, and 850 kV/cm, respectively. The current-voltage (I-V) characteristics of all samples (Fig. S4) reveal consistently low leakage currents across the measured bias range. In addition, according to previous studies, modifications in the band structure contribute to the enhancement of E b [ 25 ]. To further elucidate the underlying mechanism for the improved E b , UV-Vis spectroscopy was conducted (Fig. 3 (b)). The optical E g increases from 2.65 eV for Y0 to 2.73 eV for Y4, indicating that charge carrier migration must overcome a higher energy barrier. This widening of the E g raises the activation energy for carrier transport, effectively suppressing electrical conduction and allowing the ceramic to withstand higher applied electric fields, thereby leading to superior ESPs[ 26 ]. Figure 3 (c) shows the impedance spectra, revealing that the Y4 ceramics has a significantly higher total resistance than Y0 ceramics. The Y0 ceramics exhibits two capacitive arcs, corresponding to grains and grain boundaries responses, whereas the Y4 ceramics displays a single capacitive arc[ 27 ]. This behavior results from the formation of a high-resistance pyrochlore phase in the Y4 ceramics. The resistance of this phase exceeds the combined resistance of the grains and grain boundaries of Y0 ceramics, thereby dominating the overall impedance response [ 28 ]. To elucidate the intrinsic correlation between the dielectric breakdown behavior and the composite microstructure of PLZT- x wt% Y 2 O 3 ceramics, phase-field simulations were conducted [ 21 , 24 – 26 , 29 , 30 ].The experimentally measured SEM grain morphology from Fig. 3 (d) and (f) was used as the input microstructure for the phase simulations. In contrast to the single-pole concentration of electric potential in the pure perovskite Y0 ceramics (Fig. 3 (e)). When the breakdown path encounters the Y 2 Zr 2 O 7 grains, it hinders the electrical breakdown process (Fig. 3 (f)). This uniform distribution originates from the dual-phase grains characterized by low ε r and weak polarization. These features effectively impede the propagation of conductive pathways and suppress the localization of high electric fields. Consequently, under identical voltage conditions, the Y4 ceramics exhibits superior breakdown resistance, and reduced susceptibility to failure, thereby achieving a higher E b [ 31 , 32 ]. The dielectric temperature spectra of PLZT- x wt% Y 2 O 3 ceramics measured at 100 kHz are presented in Fig. 4 (a). All compositions exhibit distinct dielectric peaks. With increasing Y 2 O 3 content, the dielectric response evolves from three well-defined peaks in the Y0 ceramics to a single broadened peak[ 33 ], which is observed across the Y2 to Y8 ceramics. The progressive broadening of the dielectric peaks reflects characteristic diffuse phase transition behavior, which can be attributed to enhanced ionic disorder resulting from the random distribution of cations within the solid solution[ 34 ]. At elevated temperatures, the tan δ of PLZT- x wt% Y 2 O 3 ceramics shows a marked decrease. This improvement is likely due to the enhanced high‑temperature stability and the reduced high-temperature dielectric loss of the matrix imparted by the secondary phase [ 35 ]. The P - E loops characteristics of PLZT- x wt% Y 2 O 3 ceramics under 400 kV/cm are shown in Fig. 4 (b). A marked decrease in the polarization intensity of PLZT- x wt% Y 2 O 3 ceramics can be observed, and the reduction is similar to the proportional increase of the second phase. For example, the P max values of Y0, Y2, Y4, Y6, and Y8 ceramics are 52.7 C/cm 2 , 40.8 C/cm 2 , 25.2 µC/cm 2 , 15.9 µC/cm 2 , and 14.8 µC/cm 2 under 400 kV/cm, respectively. Therefore, the decrease in P max can be attributed to the incorporation of the cubic Y 2 Zr 2 O 7 phase, which possesses a highly symmetric structure and exhibits neither FE nor AFE ordering, thus contributing no spontaneous polarization. Furthermore, in Fig. 4 (c), the current peak in the I - E loops shifts toward higher electric fields, accompanied by a decrease in dielectric peak intensity and a broadening of peak width. These changes indicate that increasing the Y 2 Zr 2 O 7 content modulates the phase behavior, suppresses intense strain generation, and delays polarization saturation [ 36 ]. Figure 4 (d) and (e) present the P - E loops and ESPs of PLZT- x wt% Y 2 O 3 ceramics. This improvement arises from the synergistic effect between enhanced relaxation behavior and increased E b , resulting in a high W rec of 14.5 J/cm 3 and an η of 85.7%. A comparative analysis with other ceramics systems (Fig. 4 (f)) confirms the superior overall ESPs of Y4 ceramics, further supported by a comprehensive evaluation of its efficiency and ESPs [ 1 , 3 – 6 , 9 , 19 , 20 , 37 , 38 ]. For dielectric ceramic capacitors, the ability to withstand harsh operating conditions is critically important in practical applications. The temperature, frequency, and cycling stability of the Y4 ceramics were systematically evaluated through P ‑ E loops measurements, as shown in Fig. 5 (a) ~ (c). It can be seen that the Y4 ceramics exhibits pronounced temperature dependence over the range from 30 o C to 150 o C. With increasing temperature, this accumulated thermal energy facilitates electric domain switching, promoting the AFE-to-FE phase transition and resulting in a continuous rise in P max from 19.4 µC/cm 2 (30 o C) to 31.4 µC/cm 2 (150 o C). Accordingly, the W rec increases from 5.03 J/cm 3 at 30 o C to 7.61 J/cm 3 at 120 o C (Fig. 5 (d)). This demonstrates that Y4 ceramic can deliver enhanced ESPs at elevated temperatures (90–150 o C). The Y4 ceramics also exhibits excellent stability over a broad frequency range from 1 Hz to 1000 Hz, with only an 8% variation in its W rec , as shown in Fig. 5 (e). The ESPs remains highly stable, which is a critical advantage for high-frequency pulse power systems. To assess the cycling stability of the Y4 ceramics, Fig. 5 (f) presents the evolution of the W rec and η calculated by P - E loops after 10 4 cycles under an applied electric field of 300 kV/cm. The Y4 ceramic exhibits excellent cycling stability after 10 4 cycles with 12.6% variation in W rec . To assess its viability for pulsed power systems, the charge-discharge performance of the Y4 ceramics was investigated. Room-temperature tests were conducted under overdamped (200 Ω) and underdamped circuit conditions. As shown in Fig. 6 (a) and (b), the underdamped discharge current increases with the applied electric field. The maximum current ( I max ) of 18.6 A, current density ( C D = I max / S ) of 2369.4 A/cm 2 , and a power density ( P D = E × I max / S ) of 462 MW/cm 3 are achieved in the Y4 ceramic at 390 kV/cm. Meanwhile, the overdamped discharge curves in Fig. 6 (c) and (d) demonstrate an exceptionally rapid energy release. The discharge speed is quantified by t 0.9 , the time to release 90% of the total discharge energy density ( W dis ), calculated as follows:[ 39 – 42 ]: $$\:\begin{array}{c}{\text{W}}_{\text{dis}}\text{}\text{=}\text{}\frac{\text{R}\int\:{\text{i}}^{\text{2}}\left(\text{t}\right)\text{dt}}{\text{V}}\#\left(4\right)\end{array}$$ where V represents sample volume, and R represents load resistance (200 Ω). It can be seen that the W dis is 2.14 J/cm 3 at 430 kV/cm, and a fast discharge time of t 0.9 = 22.6 ns is obtained in Y4 ceramic. These results indicate that rare earth-modified PLZT ceramics possess outstanding ESPs, positioning them as a competitive candidate for pulsed powerapplications. \(\:\:\) 4. Conclusion This work successfully developed a Pb 0.94 La 0.04 Zr 0.99 Ti 0.01 O 3 - x wt% Y 2 O 3 (PLZT- x wt% Y 2 O 3 ) composite ceramics for dielectric energy storage. Increasing the Y 2 O 3 content x systematically enhances the E b of the PLZT matrix and promotes the evolution toward a two-phase heterostructure composed of perovskite (PLZT) and pyrochlore (Y 2 Zr 2 O 7 ) phases. Y4 ceramic achieves a large W rec of 14.5 J/cm 3 under a high E b of 570 kV/cm, together with excellent stability over a wide frequency range (1 ~ 1000 Hz) and more than 10 4 charge-discharge cycles. It also delivers a high P D of 462 MW/cm 3 , a large C D of 2369.4 C/cm 2 , and an ultrafast discharge response ( t 0.9 = 22.6 ns). The rationally designed dual‑phase heterostructure in Y4 ceramics enables exceptional integrated performance for pulsed‑power systems, thereby paving the way for a new design paradigm in high‑performance energy‑storage ceramics. Declarations Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper. Author Contribution Lei Cao: conceptualization, investigation, validation, methodology, writing - original draft. Ye Zhao: methodology, conceptualization, writing - reviewing and editing, project administration. Bowen Huang: investigation, formal analysis. Tianci Yang: investigation, formal analysis. Chenglong Jiang: investigation, formal analysis. Pei Han: investigation, formal analysis, writing - reviewing and editing. Rong Ma: investigation, formal analysis. Chunxiao Lu: investigation, formal analysis. Fen Zhao: investigation, formal analysis. Liwen Zhang: investigation, formal analysis. Yong Li: methodology, conceptualization, project administration. Acknowledgements This work was supported by the Scientific and Technological Development Foundation of the Central Guidance Local (2025ZY0168), the Natural Science Foundation of Inner Mongolia Autonomous Region (2024MS05024, 2024MS05016, 2024FX14), the Innovation Platform Construction Plan in the Inner Mongolia Autonomous Region (2025KYPT0129), and First-Class Discipline Research Special Project (YLXKZX-NKD-042). Data Availability The data that support the findings of this study are available from the corresponding author upon reasonable request. References P.-Z. Ge, X.-G. Tang, K. Meng, X.-X. Huang, S.-F. Li, Q.-X. Liu, Y.-P. Jiang, Energy storage density and charge-discharge properties of Pb x Hf 1-x SnO 3 antiferroelectric ceramics. Chem. Eng. J. 429 , 132540 (2022). http://dx.doi.org/10.1016/j.cej.2021.132540 J. Liu, Q. Chai, C. Yang, Y. Wang, Z. Peng, X. Chao, Z. 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Ge, F. Zhang, F. Yan, J. Lin, L. Tang, M. Yang, Z. Pan, X. Wei, B. Shen, Z. Liu, J. Zhai, Embedding Plate-Like Pyrochlore in Perovskite Phase to Enhance Energy Storage Performance of BNT‐Based Ceramic Capacitors. Adv. Energy Mater. 15 (12) (2024). http://dx.doi.org/10.1002/aenm.202403926 N. Luo, X. He, C. Xu, Z. Chen, K. Zhao, Z. Cen, X. Chen, D. Shan, Y. Liu, Z. Liu, H. Xie, Y. Zhu, H. Huang, J.F. Li, S. Zhang, Ordering-Structured Antiferroelectric Composite Ceramics for Energy Storage Applications. Adv. Mater. 37 (11) (2025). http://dx.doi.org/10.1002/adma.202420258 F. Yang, Y. Bao, B. Zeng, J. Wu, X. Li, Y. Sun, Y. Chen, G. Wang, Excellent energy storage properties in ZrO 2 toughened Ba 0.55 Sr 0.45 TiO 3 -based relaxor ferroelectric ceramics via multi-scale synergic regulation. Chem. Eng. J. 493 (2024). http://dx.doi.org/10.1016/j.cej.2024.152624 X. Li, Z. Dai, X. Li, C. Liu, Y. Zheng, Y. Zhang, S. Gu, X. Ren, Dual-doping strategy for enhancement of energy storage properties in Bi 0.5 Na 0.5 TiO 3 -based ceramics. J. Alloys Compd. 1048 (2025). http://dx.doi.org/10.1016/j.jallcom.2025.185245 R.T. Parayil, S.K. Gupta, K. Sudarshan, B.S. Naidu, G.D. Patra, M. Mohapatra, Tweaking the structure and symmetry of Y 2 B 2 O 7 :Eu 3+ by B-site engineering for efficient and thermally stable phosphor: Y 2 Zr 2 O 7 versus Y 2 Ge 2 O 7 . Mater. Res. Bull. 180 (2024). http://dx.doi.org/10.1016/j.materresbull.2024.113039 R. Xue, X. Liu, Y. Yang, X. Zhu, H. Wang, Enhanced energy storage density and efficiency in A/B-site-engineered silver niobate ceramics. Ceram. Int. 51 (23), 39549–39557 (2025). http://dx.doi.org/10.1016/j.ceramint.2025.06.190 X. Xiong, H. Liu, J. Zhang, L.L. da Silva, Z. Sheng, Y. Yao, G. Wang, M. Hinterstein, S. Zhang, J. Chen, Ultrahigh Energy-Storage in Dual‐Phase Relaxor Ferroelectric Ceramics. Adv. Mater. 36 (48) (2024). http://dx.doi.org/10.1002/adma.202410088 D. Li, D. Zhou, D. Wang, W. Zhao, Y. Guo, Z. Shi, T. Zhou, S.K. Sun, C. Singh, S. Trukhanov, A.S.B. Sombra, Lead-Free Relaxor Ferroelectric Ceramics with Ultrahigh Energy Storage Densities via Polymorphic Polar Nanoregions Design. Small. 19 (8) (2022). http://dx.doi.org/10.1002/smll.202206958 H.-. Lian, M. Shi, S. Lv, L.-. Liu, X.-. Chen, Dielectric, ferroelectric, and energy storage properties of BNBTA- x SLZT lead-free ceramics. J. Eur. Ceram. Soc. 45 (6), 117219 (2025). http://dx.doi.org/10.1016/j.jeurceramsoc.2025.117219 C. Wang, J. Hao, L. Duan, D. Zhao, Y. Ma, J. Zhang, P. Ma, D. Han, F. Meng, Energy storage performance with ultrahigh energy density and power density of Ba 0.85 Ca 0.15 Zr 0.1 Ti 0.9 O 3 -based lead-free ceramics through synergistic optimization. Ceram. Int. 51 (21), 35133–35143 (2025). http://dx.doi.org/10.1016/j.ceramint.2025.05.237 C. Liu, Z. Dai, Y. Zheng, X. Li, R. Dai, Y. Liu, W. Liu, S. Zhou, S. Gu, M. Fang, X. Ren, Simultaneous enhancement of the energy storage, transparency, and hardness properties of K 0.5 Na 0.5 NbO 3 -based ceramics via a synergistic optimization strategy. J. Mater. Chem. A 47 , 41365–41374 (2025). http://dx.doi.org/10.1039/d5ta06456b K. Ma, J. Cui, J. Li, X. Zhang, X. Han, L. Dong, P. Li, L. Wu, X. Qi, Multiple collaborative optimization strategy regulates tungsten bronze ceramics to achieve efficient energy storage performance. J. Energy Storage. 134 , 118203 (2025). http://dx.doi.org/10.1016/j.est.2025.118203 Additional Declarations No competing interests reported. Supplementary Files SupportingInformation.docx Cite Share Download PDF Status: Posted Version 1 posted You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. 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Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-9095268","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":610160724,"identity":"15f439b1-41f3-4a23-932a-3a4d7ce53511","order_by":0,"name":"Lei Cao","email":"","orcid":"","institution":"Inner Mongolia University of Science and Technology","correspondingAuthor":false,"prefix":"","firstName":"Lei","middleName":"","lastName":"Cao","suffix":""},{"id":610160726,"identity":"01d20804-cb49-47ef-a189-036da058223d","order_by":1,"name":"Bowen Huang","email":"","orcid":"","institution":"Inner Mongolia University of Science and 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13:53:51","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-9095268/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-9095268/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":107359241,"identity":"12c21e1d-007b-49ca-a994-2be8e54bb633","added_by":"auto","created_at":"2026-04-20 17:47:08","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":532808,"visible":true,"origin":"","legend":"\u003cp\u003eSchematic diagram of strategies for improving the comprehensive ESPs of PLZT by constructing composite ceramics\u003c/p\u003e","description":"","filename":"1.png","url":"https://assets-eu.researchsquare.com/files/rs-9095268/v1/3949b7c2ab7464632c19c79e.png"},{"id":107488653,"identity":"3d0f51b3-feae-4ab1-9d71-8f4a10a0544c","added_by":"auto","created_at":"2026-04-22 02:45:27","extension":"jpg","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":236656,"visible":true,"origin":"","legend":"\u003cp\u003e(a) XRD pattern of PLZT\u003cem\u003e- x\u003c/em\u003e wt%Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e ceramics; (b) The Rietveld refinement XRD patterns of Y0 and Y4 over 20\u003csup\u003eo\u003c/sup\u003e to 80\u003csup\u003eo\u003c/sup\u003e; (c) Phase proportion of PLZT\u003cem\u003e- x\u003c/em\u003e wt% Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e ceramics; (d) Raman spectra of Y0 and Y4 ceramics at room temperature; (e) BSE image and EDS image of Y0 ceramics; (f) BSE image and EDS image of Y4 ceramics.\u003c/p\u003e","description":"","filename":"2.jpg","url":"https://assets-eu.researchsquare.com/files/rs-9095268/v1/aefcc118fc86f2a4be96a538.jpg"},{"id":107359243,"identity":"5d0ffb0e-503e-42bf-830c-3f8cc05fb15c","added_by":"auto","created_at":"2026-04-20 17:47:08","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":1426318,"visible":true,"origin":"","legend":"\u003cp\u003e(a) Weibull distribution of \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e for PLZT- \u003cem\u003ex\u003c/em\u003e wt% Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e ceramics; (b) Tauc plot of PLZT- \u003cem\u003ex\u003c/em\u003e wt% Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e ceramics; (c) Impedance diagrams of Y0 and Y4 ceramics; (d) and (e) BSE image and EDS image of Y0 and Y4 ceramics; (f) and (g) Analog diagrams of Y4 ceramics.\u003c/p\u003e","description":"","filename":"3.png","url":"https://assets-eu.researchsquare.com/files/rs-9095268/v1/1a2ba609335f9f140e273f9c.png"},{"id":107488656,"identity":"d4028e60-480c-486f-9391-817f9b2590e7","added_by":"auto","created_at":"2026-04-22 02:45:28","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":392396,"visible":true,"origin":"","legend":"\u003cp\u003e(a) dielectric temperature spectra of PLZT- \u003cem\u003ex\u003c/em\u003e wt% Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e ceramics; (b) \u003cem\u003eP\u003c/em\u003e-\u003cem\u003eE\u003c/em\u003e loops of PLZT- \u003cem\u003ex\u003c/em\u003e wt% Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e ceramics under the same electric field; (c) \u003cem\u003eI\u003c/em\u003e-\u003cem\u003eE\u003c/em\u003e loops of PLZT- \u003cem\u003ex\u003c/em\u003e wt% Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e ceramics at \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e; (d) \u003cem\u003eP\u003c/em\u003e-\u003cem\u003eE\u003c/em\u003e loops of PLZT- \u003cem\u003ex\u003c/em\u003e wt% Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e ceramics at \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e; (e) Comparison of \u003cem\u003eW\u003c/em\u003e\u003csub\u003etot\u003c/sub\u003e, \u003cem\u003eW\u003c/em\u003e\u003csub\u003erec\u003c/sub\u003e and \u003cem\u003eh\u003c/em\u003e of PLZT- \u003cem\u003ex\u003c/em\u003e wt% Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e ceramics; (f) Comparison of \u003cem\u003eP\u003c/em\u003e\u003csub\u003emax\u003c/sub\u003e, \u003cem\u003eP\u003c/em\u003e\u003csub\u003er\u003c/sub\u003e and Δ\u003cem\u003eP\u003c/em\u003e for PLZT- \u003cem\u003ex\u003c/em\u003e wt% Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e ceramics.\u003c/p\u003e","description":"","filename":"4.png","url":"https://assets-eu.researchsquare.com/files/rs-9095268/v1/d283aa3646c863e37e62478b.png"},{"id":107359245,"identity":"bd9895ae-666b-4e10-ac49-00b186bafdf2","added_by":"auto","created_at":"2026-04-20 17:47:08","extension":"png","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":323882,"visible":true,"origin":"","legend":"\u003cp\u003e(a) \u003cem\u003eP\u003c/em\u003e-\u003cem\u003eE\u003c/em\u003e loops of Y4 ceramics at different temperatures at 400kV/cm and variations in \u003cem\u003eW\u003c/em\u003e\u003csub\u003erec\u003c/sub\u003e and \u003cem\u003eh\u003c/em\u003e with temperature; (b) \u003cem\u003eP\u003c/em\u003e-\u003cem\u003eE\u003c/em\u003e loops of Y4 ceramics at different frequencies under 400 kV/cm conditions and variations of \u003cem\u003eW\u003c/em\u003e\u003csub\u003erec\u003c/sub\u003e and \u003cem\u003eh\u003c/em\u003e with frequency; (c) \u003cem\u003eP\u003c/em\u003e-\u003cem\u003eE\u003c/em\u003e loops of Y4 ceramics at 300 kV/cm with different cycles and variations of \u003cem\u003eW\u003c/em\u003e\u003csub\u003erec\u003c/sub\u003e and \u003cem\u003eh\u003c/em\u003e with cycles.\u003c/p\u003e","description":"","filename":"5.png","url":"https://assets-eu.researchsquare.com/files/rs-9095268/v1/5e5e4a53ed57c860726d2813.png"},{"id":107486605,"identity":"56d6a5fc-94fe-4b74-a05f-e0cd1108619d","added_by":"auto","created_at":"2026-04-22 02:38:31","extension":"png","order_by":6,"title":"Figure 6","display":"","copyAsset":false,"role":"figure","size":161785,"visible":true,"origin":"","legend":"\u003cp\u003e(a) Pulse charge-discharge performance of Y4 ceramic under different electric fields in the underdamped state; (b) Y4 ceramic \u003cem\u003eI\u003c/em\u003e\u003csub\u003emax\u003c/sub\u003e, \u003cem\u003eP\u003c/em\u003e\u003csub\u003eD\u003c/sub\u003e, \u003cem\u003eC\u003c/em\u003e\u003csub\u003eD\u003c/sub\u003e tests; (c) Pulse charge-discharge performance of Y4 ceramic under different electric fields in overdamped state; (d) Calculate the variation of \u003cem\u003eW\u003c/em\u003e\u003csub\u003ed\u003c/sub\u003e and \u003cem\u003et\u003c/em\u003e\u003csub\u003e0.9\u003c/sub\u003e over time by integration\u003c/p\u003e","description":"","filename":"6.png","url":"https://assets-eu.researchsquare.com/files/rs-9095268/v1/a5cf784fd71398c810fb240b.png"},{"id":108976549,"identity":"6cd94d1b-84ed-4317-a6a9-4db2816ac676","added_by":"auto","created_at":"2026-05-11 11:25:18","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":3329746,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-9095268/v1/a2924d23-2690-4f62-ac26-c7f37c3a6b2d.pdf"},{"id":107359240,"identity":"49959bb9-a4dd-41d8-9b74-328f5b51da61","added_by":"auto","created_at":"2026-04-20 17:47:08","extension":"docx","order_by":0,"title":"","display":"","copyAsset":false,"role":"supplement","size":1551521,"visible":true,"origin":"","legend":"","description":"","filename":"SupportingInformation.docx","url":"https://assets-eu.researchsquare.com/files/rs-9095268/v1/dfe344ea01a7a0c0bf562559.docx"}],"financialInterests":"No competing interests reported.","formattedTitle":"\u003cp\u003eUltrahigh energy storage performance in Pb\u003csub\u003e0.94\u003c/sub\u003eLa\u003csub\u003e0.04\u003c/sub\u003eZr\u003csub\u003e0.99\u003c/sub\u003eTi\u003csub\u003e0.01\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e ceramics via introducing pyrochlore phase Y\u003csub\u003e2\u003c/sub\u003eZr\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e7\u003c/sub\u003e\u003c/p\u003e","fulltext":[{"header":"1. Introduction","content":"\u003cp\u003eCeramic capacitors exhibit broad application prospects in electric vehicles, pulse power systems, and other fields due to their excellent charge-discharge rates and high power density (\u003cem\u003eP\u003c/em\u003e\u003csub\u003eD\u003c/sub\u003e)[\u003cspan additionalcitationids=\"CR2\" citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR3\" class=\"CitationRef\"\u003e3\u003c/span\u003e]. However, the relatively low energy storage density remains a key bottleneck limiting their miniaturization and integration. Therefore, improving energy storage properties (ESPs) is of significant scientific importance and practical value. In general, the total energy storage density (\u003cem\u003eW\u003c/em\u003e\u003csub\u003etot\u003c/sub\u003e), recoverable energy storage density (\u003cem\u003eW\u003c/em\u003e\u003csub\u003erec\u003c/sub\u003e) and energy storage efficiency (\u003cem\u003e\u0026eta;\u003c/em\u003e) of dielectric ceramic capacitors can be calculated using the following formulas[\u003cspan citationid=\"CR4\" class=\"CitationRef\"\u003e4\u003c/span\u003e]:\u003c/p\u003e\n\u003cdiv id=\"Equa\" class=\"Equation\"\u003e\n \u003cdiv format=\"TEX\" class=\"mathdisplay\" id=\"FileID_Equa\" name=\"EquationSource\"\u003e$$\\:\\begin{array}{c}{\\text{W}}_{\\text{tot}}\\text{}\\text{=}\\text{}{\\int\\:}_{\\text{0}}^{{\\text{P}}_{\\text{max}}}\\text{EdP}\\#\\left(1\\right)\\end{array}$$\u003c/div\u003e\n\u003c/div\u003e\n\u003cdiv id=\"Equb\" class=\"Equation\"\u003e\n \u003cdiv format=\"TEX\" class=\"mathdisplay\" id=\"FileID_Equb\" name=\"EquationSource\"\u003e$$\\:\\begin{array}{c}{\\text{W}}_{\\text{rec}}\\text{}\\text{=}\\text{}{\\int\\:}_{{\\text{P}}_{\\text{r}}}^{{\\text{P}}_{\\text{max}}}\\text{EdP}\\#\\left(2\\right)\\end{array}$$\u003c/div\u003e\n\u003c/div\u003e\n\u003cdiv id=\"Equc\" class=\"Equation\"\u003e\n \u003cdiv format=\"TEX\" class=\"mathdisplay\" id=\"FileID_Equc\" name=\"EquationSource\"\u003e$$\\:\\begin{array}{c}\\text{ɳ}\\text{=}\\text{}\\frac{{\\text{W}}_{\\text{rec}}}{{\\text{W}}_{\\text{tot}}}\\text{\u0026times;}\\text{100}\\text{%}\\#\\left(3\\right)\\end{array}$$\u003c/div\u003e\u003c/div\u003e\u003cp\u003ewhere \u003cem\u003eE\u003c/em\u003e, \u003cem\u003eP\u003c/em\u003e\u003csub\u003er\u003c/sub\u003e, and \u003cem\u003eP\u003c/em\u003e\u003csub\u003emax\u003c/sub\u003e denote as the applied electric field, remanent polarization, and maximum polarization, respectively. The formulas reveal that achieving a high \u003cem\u003eW\u003c/em\u003e\u003csub\u003erec\u003c/sub\u003e necessitates concurrently high \u003cem\u003eP\u003c/em\u003e\u003csub\u003emax\u003c/sub\u003e, low \u003cem\u003eP\u003c/em\u003e\u003csub\u003er\u003c/sub\u003e and high breakdown field (\u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e). Among these, pursuing \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e optimization emerges as a particularly effective strategy, as the improvement from polarization enhancement alone is intrinsically constrained[\u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e].\u003c/p\u003e\u003cp\u003ePbZrO\u003csub\u003e3\u003c/sub\u003e (PZ) -based antiferroelectric (AFE) ceramics are considered one of the most promising energy storage dielectric ceramics for achieving high \u003cem\u003eW\u003c/em\u003e\u003csub\u003erec\u003c/sub\u003e due to their unique double hysteresis loops and high \u003cem\u003eP\u003c/em\u003e\u003csub\u003emax\u003c/sub\u003e and near-zero \u003cem\u003eP\u003c/em\u003e\u003csub\u003er\u003c/sub\u003e[\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e]. The ESPs of PZ-based AFE materials are primarily constrained by their low \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e. Consequently, rare-earth ion doping has been widely adopted as a feasible strategy to enhance \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e and thereby improve ESPs[\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e]. For example, Yang et al. demonstrated that Nd\u003csup\u003e3+\u003c/sup\u003e doping stabilized the AFE phase in a Pb\u003csub\u003e0.98\u003c/sub\u003eSr\u003csub\u003e0.02\u003c/sub\u003eZr\u003csub\u003e0.75\u003c/sub\u003eSn\u003csub\u003e0.25\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e (PSrZS) ceramics, increasing its \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e from 350 kV/cm to 540 kV/cm and resulting in a high \u003cem\u003eW\u003c/em\u003e\u003csub\u003erec\u003c/sub\u003e of 14.21 J/cm\u003csup\u003e3\u003c/sup\u003e with \u003cem\u003e\u0026eta;\u003c/em\u003e of 87.35%[\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e]. In addition to ion doping, constructing dual-phase composite ceramics is also an effective strategy to improve the breakdown characteristics of dielectric ceramics[\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e]. For example, Pan et al. introduced the pyrochlore Sm\u003csub\u003e2\u003c/sub\u003eSn\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e7\u003c/sub\u003e into a Bi\u003csub\u003e0.5\u003c/sub\u003eNa\u003csub\u003e0.5\u003c/sub\u003eTiO\u003csub\u003e3\u003c/sub\u003e (BNT) -based perovskite matrix, raising the \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e from 220 to 700 kV/cm and achieving a \u003cem\u003eW\u003c/em\u003e\u003csub\u003erec\u003c/sub\u003e of 9.91 J/cm\u003csup\u003e3\u003c/sup\u003e with \u003cem\u003e\u0026eta;\u003c/em\u003e of 87.01%[\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e]. Such enhanced ESPs are attributed to the existence of pyrochlore phase in perovskite matrix, which possesses a low dielectric constant (\u003cem\u003e\u0026epsilon;\u003c/em\u003e\u003csub\u003er\u003c/sub\u003e), wide bandgap (\u003cem\u003eE\u003c/em\u003e\u003csub\u003eg\u003c/sub\u003e), low dielectric loss (tan\u003cem\u003e\u0026delta;\u003c/em\u003e), and high stability[\u003cspan additionalcitationids=\"CR12\" citationid=\"CR11\" class=\"CitationRef\"\u003e11\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e13\u003c/span\u003e]. Therefore, constructing a composite structure by introducing a pyrochlore phase (Y\u003csub\u003e2\u003c/sub\u003eZr\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e7\u003c/sub\u003e) into perovskite dielectric ceramics is a promising strategy to significantly enhance ESPs, offering broad application prospects.\u003c/p\u003e\u003cp\u003eY\u003csub\u003e2\u003c/sub\u003eZr\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e7\u003c/sub\u003e is a pyrochlore phase transparent ceramic with a low \u003cem\u003e\u0026epsilon;\u003c/em\u003e\u003csub\u003er\u003c/sub\u003e (~\u0026thinsp;27), wide \u003cem\u003eE\u003c/em\u003e\u003csub\u003eg\u003c/sub\u003e (~\u0026thinsp;4.5 eV), low tan\u003cem\u003e\u0026delta;\u003c/em\u003e (~\u0026thinsp;0.001), and high thermal resistance (1.2\u0026thinsp;~\u0026thinsp;1.3 W/(m\u0026middot;k)). While currently utilized mainly in phosphors and photochromism applications, distinctive dielectric properties also render it a promising candidate for energy storage applications[\u003cspan additionalcitationids=\"CR15 CR16 CR17\" citationid=\"CR14\" class=\"CitationRef\"\u003e14\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR18\" class=\"CitationRef\"\u003e18\u003c/span\u003e]. Previous studies indicate that doping Y\u003csup\u003e3+\u003c/sup\u003e into the A-site can induce local chemical disorder, disrupt the original long-range ferroelectric order of the PZ-based ceramics, and promote a transition to a diffuse relaxor state. Simultaneously, it helps to reduce oxygen vacancy concentration, refine grain size, and enhance \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e[\u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e19\u003c/span\u003e]. In this work, a series of Pb\u003csub\u003e0.94\u003c/sub\u003eLa\u003csub\u003e0.04\u003c/sub\u003eZr\u003csub\u003e0.99\u003c/sub\u003eTi\u003csub\u003e0.01\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e (PLZT) - \u003cem\u003ex\u003c/em\u003e wt% Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e ceramics were designed by introducing \u003cem\u003ex\u003c/em\u003e wt% Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e at the initial mixing stage. This non-equivalent doping strategy promotes the directional formation of a secondary phase within the PLZT matrix. Consequently, it enhances the stability of the AFE state and simultaneously improves the \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e, leading to excellent overall ESPs. This work offers a promising composite ceramic candidate for pulsed power systems.\u003c/p\u003e"},{"header":"2. Experimental Section","content":"\u003cp\u003eAntiferroelectric ceramics with the composition of Pb\u003csub\u003e0.94\u003c/sub\u003eLa\u003csub\u003e0.04\u003c/sub\u003eZr\u003csub\u003e0.99\u003c/sub\u003eTi\u003csub\u003e0.01\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e- \u003cem\u003ex\u003c/em\u003e wt%Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e with \u003cem\u003ex\u003c/em\u003e\u0026thinsp;=\u0026thinsp;0, 2, 4, 6, and 8 were prepared by a tape-casting. These samples are accordingly designated as Y0, Y2, Y4, Y6 and Y8. The starting materials are lead tetroxide (Pb\u003csub\u003e3\u003c/sub\u003eO\u003csub\u003e4\u003c/sub\u003e, 95.0%), yttrium oxide (Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e, 99.9%), zirconium dioxide (ZrO\u003csub\u003e2\u003c/sub\u003e, 99.0%), titanium dioxide (TiO\u003csub\u003e2\u003c/sub\u003e, 99.5%), lanthanum oxide (La\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e, 99.9%). PLZT (Pb\u003csub\u003e0.94\u003c/sub\u003eLa\u003csub\u003e0.04\u003c/sub\u003eZr\u003csub\u003e0.99\u003c/sub\u003eTi\u003csub\u003e0.01\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e) were weighed according to the stoichiometric ratio, but yttrium oxide is doped in proportion to the mass of the corresponding powder. All raw materials ball milled in alcohol for 24 h. The mixture was calcined at 900 \u003csup\u003eo\u003c/sup\u003eC for 2 h, followed by grinding and a second 24 h ball-milling. After drying and sieving, the powder was shaped via tape-casting, subsequently air-dried, and densified through sequential hot pressing and cold isostatic pressing. Organic components were removed at 600 \u003csup\u003eo\u003c/sup\u003eC for 5 h. The samples were sintered at 1160 \u003csup\u003eo\u003c/sup\u003eC for 3 h, polished to a thickness of ~\u0026thinsp;70 \u0026micro;m, and coated with 1 mm-diameter gold electrodes via ion suppering for electrical properties.\u003c/p\u003e \u003cp\u003eThe crystal structure was characterized using X-ray diffraction (XRD; Bruker D8 Advance) with Cu K\u003cem\u003eα\u003c/em\u003e radiation. The obtained diffraction patterns were refined using the Rietveld method in GSAS-II software. Microstructure analysis was conducted using a scanning electron microscope (SEM; Thermo Fisher MIRA3) operated in backscattered electron (BSE) mode. The impedance spectrum was measured using an impedance analyzer (Agilent E4990A). The polarization-electric field (\u003cem\u003eP\u003c/em\u003e-\u003cem\u003eE\u003c/em\u003e) hysteresis loops and current-electric field (\u003cem\u003eI\u003c/em\u003e-\u003cem\u003eE\u003c/em\u003e) curve loops were measured using a ferroelectric testing system integrated with a temperature-controlled probe station (Radiant Technologies) at 10 Hz. The charge-discharge performance was evaluated using a dedicated pulse power platform (Gogo Instruments CFD137005) connected to a DC power supply (ENTAI ET2671A).\u003c/p\u003e"},{"header":"3. Results and Discussion","content":"\u003cp\u003eFigure\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e(a) presents the XRD pattern of the PLZT- \u003cem\u003ex\u003c/em\u003e wt% Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e ceramic. The main crystalline phase corresponds to a typical perovskite structure (PDF# 97-016-6843) with an orthorhombic symmetry. With increasing Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e content, diffraction peaks corresponding to the cubic pyrochlore phase Y\u003csub\u003e2\u003c/sub\u003eZr\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e7\u003c/sub\u003e (PDF# 97-015-3818) gradually emerge, and their intensities progressively increase. The results indicate that excessive Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e doping exceeds the solid solubility limit in the PLZT matrix, leading to the precipitation of the secondary phase[\u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e]. To quantify the relative content of the perovskite and pyrochlore phases, the Rietveld refinement was conducted. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e(b), the Rietveld refinement results of Y0 and Y4 ceramics indicate that all samples exhibit a typical perovskite structure, and the content of pyrochlore phase monotonically increases with the increase of Y\u003csup\u003e3+\u003c/sup\u003e content. The refinement was carried out simultaneously based on two spatial group models: orthorhombic phase Pba2 and cubic phase Fd-3m. All the samples exhibit low \u003cem\u003eR\u003c/em\u003e-factors (\u003cem\u003eR\u003c/em\u003e\u003csub\u003ewp\u003c/sub\u003e \u0026lt; 10%), and unit cell parameters for Y4 ceramics are provided in \u003cb\u003eFig. \u003cspan refid=\"MOESM1\" class=\"InternalRef\"\u003eS1\u003c/span\u003e.\u003c/b\u003e These results confirm the validity of the structural models and the reliability of the refinement, with the calculated patterns showing excellent agreement with the experimental data[\u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e]. The XRD Rietveld refinement patterns for ceramics Y2, Y6 and Y8 are provided in \u003cb\u003eFig. S2.\u003c/b\u003e It can be seen that the formation of the Y\u003csub\u003e2\u003c/sub\u003eZr\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e7\u003c/sub\u003e pyrochlore phase increases the cubic phase fraction to 8.8% in Y2 sample. With further increase in Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e addition, it reaches 48% in Y4 and eventually rises nonlinearly to 60.4% in Y8 (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e(c)). This evolution is attributed to the limited solubility of Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e in the PLZT lattice. This limited solubility disrupts the long-range ferroelectric order, thereby enhancing the relaxor behavior of the materials [\u003cspan citationid=\"CR22\" class=\"CitationRef\"\u003e22\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eTo further elucidate the influence of Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e on the structural characteristics, room-temperature Raman spectra were collected (\u003cb\u003eFig. S3\u003c/b\u003e). A detailed Gaussian-Lorentzian fitting analysis was conducted on the Raman spectra of the Y0 and Y4 samples, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e(d). The spectral features are systematically divided into three distinct regions: A-site ion vibrations (50\u0026thinsp;~\u0026thinsp;150 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e), B-O bond vibrations (150\u0026thinsp;~\u0026thinsp;450 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e), and BO\u003csub\u003e6\u003c/sub\u003e octahedral vibrations (450\u0026thinsp;~\u0026thinsp;800 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e). The Y4 sample exhibits significant spectral alterations in the low-frequency region (\u0026lt;\u0026thinsp;150 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e) compared to Y0, resulting from the perturbation of A-site vibrational modes by Y\u003csup\u003e3+\u003c/sup\u003e doping. Concurrently, the Raman peak near 220 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e shifts in position and exhibits a reduced full width at half maximum (FWHM), indicating enhanced lattice distortion [\u003cspan citationid=\"CR23\" class=\"CitationRef\"\u003e23\u003c/span\u003e]. Furthermore, in the region of 450\u0026thinsp;~\u0026thinsp;800 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, the absence of a characteristic J-fitting peak in Y4 sample suggests that the precipitation of the secondary phase enhances the structural stability of the BO\u003csub\u003e6\u003c/sub\u003e octahedra.\u003c/p\u003e \u003cp\u003eAs shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e(e) and (f), both Y0 and Y4 ceramics exhibit well-defined grain with sharp boundaries and a dense microstructure, indicating the suitability of the sintering temperature. The BSE images (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e(f)) reveal the stable coexistence of pyrochlore phase Y\u003csub\u003e2\u003c/sub\u003eZr\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e7\u003c/sub\u003e and perovskite phase PLZT in the Y4 ceramic, which has been consistently reproduced in repeated experiments. This indicates that the significant enhancement in \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e is not due to grain size effects[\u003cspan citationid=\"CR22\" class=\"CitationRef\"\u003e22\u003c/span\u003e]. To identify the composition of the second phase, energy-dispersive X-ray spectroscopy (EDS) was conducted on all samples, as shown in \u003cb\u003eFig. S4\u003c/b\u003e. The results demonstrate a distinct co-enrichment of Y\u003csup\u003e3+\u003c/sup\u003e and Zr\u003csup\u003e4+\u003c/sup\u003e ions in Y4 samples, confirming the formation of the Y\u003csub\u003e2\u003c/sub\u003eZr\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e7\u003c/sub\u003e secondary phase[\u003cspan citationid=\"CR23\" class=\"CitationRef\"\u003e23\u003c/span\u003e].\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eThe breakdown reliability was evaluated using Weibull distribution analysis, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e(a). All the PLZT- \u003cem\u003ex\u003c/em\u003e wt% Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e ceramics exhibit a Weibull modulus (\u003cem\u003eβ\u003c/em\u003e) higher than 10, indicating excellent consistency and high reliability of the \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e[\u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e]. The \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e of Y0, Y2, Y4, Y6, and Y8 ceramics are 440 kV/cm, 490 kV/cm, 570 kV/cm, 720 kV/cm, and 850 kV/cm, respectively. The current-voltage (I-V) characteristics of all samples (Fig. S4) reveal consistently low leakage currents across the measured bias range. In addition, according to previous studies, modifications in the band structure contribute to the enhancement of \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e[\u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e25\u003c/span\u003e]. To further elucidate the underlying mechanism for the improved \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e, UV-Vis spectroscopy was conducted (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e(b)). The optical \u003cem\u003eE\u003c/em\u003e\u003csub\u003eg\u003c/sub\u003e increases from 2.65 eV for Y0 to 2.73 eV for Y4, indicating that charge carrier migration must overcome a higher energy barrier. This widening of the \u003cem\u003eE\u003c/em\u003e\u003csub\u003eg\u003c/sub\u003e raises the activation energy for carrier transport, effectively suppressing electrical conduction and allowing the ceramic to withstand higher applied electric fields, thereby leading to superior ESPs[\u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e26\u003c/span\u003e]. Figure\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e(c) shows the impedance spectra, revealing that the Y4 ceramics has a significantly higher total resistance than Y0 ceramics. The Y0 ceramics exhibits two capacitive arcs, corresponding to grains and grain boundaries responses, whereas the Y4 ceramics displays a single capacitive arc[\u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e27\u003c/span\u003e]. This behavior results from the formation of a high-resistance pyrochlore phase in the Y4 ceramics. The resistance of this phase exceeds the combined resistance of the grains and grain boundaries of Y0 ceramics, thereby dominating the overall impedance response [\u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e28\u003c/span\u003e]. To elucidate the intrinsic correlation between the dielectric breakdown behavior and the composite microstructure of PLZT- \u003cem\u003ex\u003c/em\u003e wt% Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e ceramics, phase-field simulations were conducted [\u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e, \u003cspan additionalcitationids=\"CR25\" citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e26\u003c/span\u003e, \u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e, \u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e].The experimentally measured SEM grain morphology from Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e(d) and (f) was used as the input microstructure for the phase simulations. In contrast to the single-pole concentration of electric potential in the pure perovskite Y0 ceramics (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e(e)). When the breakdown path encounters the Y\u003csub\u003e2\u003c/sub\u003eZr\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e7\u003c/sub\u003e grains, it hinders the electrical breakdown process (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e(f)). This uniform distribution originates from the dual-phase grains characterized by low \u003cem\u003eε\u003c/em\u003e\u003csub\u003er\u003c/sub\u003e and weak polarization. These features effectively impede the propagation of conductive pathways and suppress the localization of high electric fields. Consequently, under identical voltage conditions, the Y4 ceramics exhibits superior breakdown resistance, and reduced susceptibility to failure, thereby achieving a higher \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e[\u003cspan citationid=\"CR31\" class=\"CitationRef\"\u003e31\u003c/span\u003e, \u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e32\u003c/span\u003e].\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eThe dielectric temperature spectra of PLZT- \u003cem\u003ex\u003c/em\u003e wt% Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e ceramics measured at 100 kHz are presented in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e(a). All compositions exhibit distinct dielectric peaks. With increasing Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e content, the dielectric response evolves from three well-defined peaks in the Y0 ceramics to a single broadened peak[\u003cspan citationid=\"CR33\" class=\"CitationRef\"\u003e33\u003c/span\u003e], which is observed across the Y2 to Y8 ceramics. The progressive broadening of the dielectric peaks reflects characteristic diffuse phase transition behavior, which can be attributed to enhanced ionic disorder resulting from the random distribution of cations within the solid solution[\u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e34\u003c/span\u003e]. At elevated temperatures, the tan\u003cem\u003eδ\u003c/em\u003e of PLZT- \u003cem\u003ex\u003c/em\u003e wt% Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e ceramics shows a marked decrease. This improvement is likely due to the enhanced high‑temperature stability and the reduced high-temperature dielectric loss of the matrix imparted by the secondary phase [\u003cspan citationid=\"CR35\" class=\"CitationRef\"\u003e35\u003c/span\u003e]. The \u003cem\u003eP\u003c/em\u003e-\u003cem\u003eE\u003c/em\u003e loops characteristics of PLZT- \u003cem\u003ex\u003c/em\u003e wt% Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e ceramics under 400 kV/cm are shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e(b). A marked decrease in the polarization intensity of PLZT- \u003cem\u003ex\u003c/em\u003e wt% Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e ceramics can be observed, and the reduction is similar to the proportional increase of the second phase. For example, the \u003cem\u003eP\u003c/em\u003e\u003csub\u003emax\u003c/sub\u003e values of Y0, Y2, Y4, Y6, and Y8 ceramics are 52.7 C/cm\u003csup\u003e2\u003c/sup\u003e, 40.8 C/cm\u003csup\u003e2\u003c/sup\u003e, 25.2 \u0026micro;C/cm\u003csup\u003e2\u003c/sup\u003e, 15.9 \u0026micro;C/cm\u003csup\u003e2\u003c/sup\u003e, and 14.8 \u0026micro;C/cm\u003csup\u003e2\u003c/sup\u003e under 400 kV/cm, respectively. Therefore, the decrease in \u003cem\u003eP\u003c/em\u003e\u003csub\u003emax\u003c/sub\u003e can be attributed to the incorporation of the cubic Y\u003csub\u003e2\u003c/sub\u003eZr\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e7\u003c/sub\u003e phase, which possesses a highly symmetric structure and exhibits neither FE nor AFE ordering, thus contributing no spontaneous polarization. Furthermore, in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e(c), the current peak in the \u003cem\u003eI\u003c/em\u003e-\u003cem\u003eE\u003c/em\u003e loops shifts toward higher electric fields, accompanied by a decrease in dielectric peak intensity and a broadening of peak width. These changes indicate that increasing the Y\u003csub\u003e2\u003c/sub\u003eZr\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e7\u003c/sub\u003e content modulates the phase behavior, suppresses intense strain generation, and delays polarization saturation [\u003cspan citationid=\"CR36\" class=\"CitationRef\"\u003e36\u003c/span\u003e]. Figure\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e(d) and (e) present the \u003cem\u003eP\u003c/em\u003e-\u003cem\u003eE\u003c/em\u003e loops and ESPs of PLZT- \u003cem\u003ex\u003c/em\u003e wt% Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e ceramics. This improvement arises from the synergistic effect between enhanced relaxation behavior and increased \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e, resulting in a high \u003cem\u003eW\u003c/em\u003e\u003csub\u003erec\u003c/sub\u003e of 14.5 J/cm\u003csup\u003e3\u003c/sup\u003e and an \u003cem\u003eη\u003c/em\u003e of 85.7%. A comparative analysis with other ceramics systems (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e(f)) confirms the superior overall ESPs of Y4 ceramics, further supported by a comprehensive evaluation of its efficiency and ESPs [\u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e, \u003cspan additionalcitationids=\"CR4 CR5\" citationid=\"CR3\" class=\"CitationRef\"\u003e3\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e, \u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e, \u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e19\u003c/span\u003e, \u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e, \u003cspan citationid=\"CR37\" class=\"CitationRef\"\u003e37\u003c/span\u003e, \u003cspan citationid=\"CR38\" class=\"CitationRef\"\u003e38\u003c/span\u003e].\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eFor dielectric ceramic capacitors, the ability to withstand harsh operating conditions is critically important in practical applications. The temperature, frequency, and cycling stability of the Y4 ceramics were systematically evaluated through \u003cem\u003eP\u003c/em\u003e‑\u003cem\u003eE\u003c/em\u003e loops measurements, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003e(a) ~ (c). It can be seen that the Y4 ceramics exhibits pronounced temperature dependence over the range from 30 \u003csup\u003eo\u003c/sup\u003eC to 150 \u003csup\u003eo\u003c/sup\u003eC. With increasing temperature, this accumulated thermal energy facilitates electric domain switching, promoting the AFE-to-FE phase transition and resulting in a continuous rise in \u003cem\u003eP\u003c/em\u003e\u003csub\u003emax\u003c/sub\u003e from 19.4 \u0026micro;C/cm\u003csup\u003e2\u003c/sup\u003e (30 \u003csup\u003eo\u003c/sup\u003eC) to 31.4 \u0026micro;C/cm\u003csup\u003e2\u003c/sup\u003e (150 \u003csup\u003eo\u003c/sup\u003eC). Accordingly, the \u003cem\u003eW\u003c/em\u003e\u003csub\u003erec\u003c/sub\u003e increases from 5.03 J/cm\u003csup\u003e3\u003c/sup\u003e at 30 \u003csup\u003eo\u003c/sup\u003eC to 7.61 J/cm\u003csup\u003e3\u003c/sup\u003e at 120 \u003csup\u003eo\u003c/sup\u003eC (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003e(d)). This demonstrates that Y4 ceramic can deliver enhanced ESPs at elevated temperatures (90\u0026ndash;150 \u003csup\u003eo\u003c/sup\u003eC). The Y4 ceramics also exhibits excellent stability over a broad frequency range from 1 Hz to 1000 Hz, with only an 8% variation in its \u003cem\u003eW\u003c/em\u003e\u003csub\u003erec\u003c/sub\u003e, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003e(e). The ESPs remains highly stable, which is a critical advantage for high-frequency pulse power systems. To assess the cycling stability of the Y4 ceramics, Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003e (f) presents the evolution of the \u003cem\u003eW\u003c/em\u003e\u003csub\u003erec\u003c/sub\u003e and \u003cem\u003eη\u003c/em\u003e calculated by \u003cem\u003eP\u003c/em\u003e-\u003cem\u003eE\u003c/em\u003e loops after 10\u003csup\u003e4\u003c/sup\u003e cycles under an applied electric field of 300 kV/cm. The Y4 ceramic exhibits excellent cycling stability after 10\u003csup\u003e4\u003c/sup\u003e cycles with 12.6% variation in \u003cem\u003eW\u003c/em\u003e\u003csub\u003erec\u003c/sub\u003e.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eTo assess its viability for pulsed power systems, the charge-discharge performance of the Y4 ceramics was investigated. Room-temperature tests were conducted under overdamped (200 Ω) and underdamped circuit conditions. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003e(a) and (b), the underdamped discharge current increases with the applied electric field. The maximum current (\u003cem\u003eI\u003c/em\u003e\u003csub\u003emax\u003c/sub\u003e) of 18.6 A, current density (\u003cem\u003eC\u003c/em\u003e\u003csub\u003eD\u003c/sub\u003e = \u003cem\u003eI\u003c/em\u003e\u003csub\u003emax\u003c/sub\u003e / \u003cem\u003eS\u003c/em\u003e) of 2369.4 A/cm\u003csup\u003e2\u003c/sup\u003e, and a power density (\u003cem\u003eP\u003c/em\u003e\u003csub\u003eD\u003c/sub\u003e = \u003cem\u003eE\u003c/em\u003e \u0026times; \u003cem\u003eI\u003c/em\u003e\u003csub\u003emax\u003c/sub\u003e / \u003cem\u003eS\u003c/em\u003e) of 462 MW/cm\u003csup\u003e3\u003c/sup\u003e are achieved in the Y4 ceramic at 390 kV/cm. Meanwhile, the overdamped discharge curves in Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003e(c) and (d) demonstrate an exceptionally rapid energy release. The discharge speed is quantified by \u003cem\u003et\u003c/em\u003e\u003csub\u003e0.9\u003c/sub\u003e, the time to release 90% of the total discharge energy density (\u003cem\u003eW\u003c/em\u003e\u003csub\u003edis\u003c/sub\u003e), calculated as follows:[\u003cspan additionalcitationids=\"CR40 CR41\" citationid=\"CR39\" class=\"CitationRef\"\u003e39\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR42\" class=\"CitationRef\"\u003e42\u003c/span\u003e]:\u003cdiv id=\"Equd\" class=\"Equation\"\u003e\u003cdiv format=\"TEX\" class=\"mathdisplay\" id=\"FileID_Equd\" name=\"EquationSource\"\u003e\n$$\\:\\begin{array}{c}{\\text{W}}_{\\text{dis}}\\text{}\\text{=}\\text{}\\frac{\\text{R}\\int\\:{\\text{i}}^{\\text{2}}\\left(\\text{t}\\right)\\text{dt}}{\\text{V}}\\#\\left(4\\right)\\end{array}$$\u003c/div\u003e\u003c/div\u003e\u003c/p\u003e \u003cp\u003ewhere \u003cem\u003eV\u003c/em\u003e represents sample volume, and \u003cem\u003eR\u003c/em\u003e represents load resistance (200 Ω). It can be seen that the \u003cem\u003eW\u003c/em\u003e\u003csub\u003edis\u003c/sub\u003e is 2.14 J/cm\u003csup\u003e3\u003c/sup\u003e at 430 kV/cm, and a fast discharge time of \u003cem\u003et\u003c/em\u003e\u003csub\u003e0.9\u003c/sub\u003e = 22.6 ns is obtained in Y4 ceramic. These results indicate that rare earth-modified PLZT ceramics possess outstanding ESPs, positioning them as a competitive candidate for pulsed powerapplications.\u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(\\:\\:\\)\u003c/span\u003e\u003c/span\u003e\u003c/p\u003e \u003cp\u003e \u003c/p\u003e"},{"header":"4. Conclusion","content":"\u003cp\u003eThis work successfully developed a Pb\u003csub\u003e0.94\u003c/sub\u003eLa\u003csub\u003e0.04\u003c/sub\u003eZr\u003csub\u003e0.99\u003c/sub\u003eTi\u003csub\u003e0.01\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e- \u003cem\u003ex\u003c/em\u003e wt% Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e (PLZT- \u003cem\u003ex\u003c/em\u003e wt% Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e) composite ceramics for dielectric energy storage. Increasing the Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e content \u003cem\u003ex\u003c/em\u003e systematically enhances the \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e of the PLZT matrix and promotes the evolution toward a two-phase heterostructure composed of perovskite (PLZT) and pyrochlore (Y\u003csub\u003e2\u003c/sub\u003eZr\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e7\u003c/sub\u003e) phases. Y4 ceramic achieves a large \u003cem\u003eW\u003c/em\u003e\u003csub\u003erec\u003c/sub\u003e of 14.5 J/cm\u003csup\u003e3\u003c/sup\u003e under a high \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e of 570 kV/cm, together with excellent stability over a wide frequency range (1\u0026thinsp;~\u0026thinsp;1000 Hz) and more than 10\u003csup\u003e4\u003c/sup\u003e charge-discharge cycles. It also delivers a high \u003cem\u003eP\u003c/em\u003e\u003csub\u003eD\u003c/sub\u003e of 462 MW/cm\u003csup\u003e3\u003c/sup\u003e, a large \u003cem\u003eC\u003c/em\u003e\u003csub\u003eD\u003c/sub\u003e of 2369.4 C/cm\u003csup\u003e2\u003c/sup\u003e, and an ultrafast discharge response (\u003cem\u003et\u003c/em\u003e\u003csub\u003e0.9\u003c/sub\u003e = 22.6 ns). The rationally designed dual‑phase heterostructure in Y4 ceramics enables exceptional integrated performance for pulsed‑power systems, thereby paving the way for a new design paradigm in high‑performance energy‑storage ceramics.\u003c/p\u003e"},{"header":"Declarations","content":"\u003cp\u003e \u003ch2\u003eDeclaration of competing interest\u003c/h2\u003e \u003cp\u003eThe authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.\u003c/p\u003e \u003c/p\u003e\u003ch2\u003eAuthor Contribution\u003c/h2\u003e\u003cp\u003eLei Cao: conceptualization, investigation, validation, methodology, writing - original draft. Ye Zhao: methodology, conceptualization, writing - reviewing and editing, project administration. Bowen Huang: investigation, formal analysis. Tianci Yang: investigation, formal analysis. Chenglong Jiang: investigation, formal analysis. Pei Han: investigation, formal analysis, writing - reviewing and editing. Rong Ma: investigation, formal analysis. Chunxiao Lu: investigation, formal analysis. Fen Zhao: investigation, formal analysis. Liwen Zhang: investigation, formal analysis. Yong Li: methodology, conceptualization, project administration.\u003c/p\u003e\u003ch2\u003eAcknowledgements\u003c/h2\u003e \u003cp\u003eThis work was supported by the Scientific and Technological Development Foundation of the Central Guidance Local (2025ZY0168), the Natural Science Foundation of Inner Mongolia Autonomous Region (2024MS05024, 2024MS05016, 2024FX14), the Innovation Platform Construction Plan in the Inner Mongolia Autonomous Region (2025KYPT0129), and First-Class Discipline Research Special Project (YLXKZX-NKD-042).\u003c/p\u003e\u003ch2\u003eData Availability\u003c/h2\u003e\u003cp\u003eThe data that support the findings of this study are available from the corresponding author upon reasonable request.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\u003cli\u003e\u003cspan\u003eP.-Z. Ge, X.-G. Tang, K. Meng, X.-X. Huang, S.-F. Li, Q.-X. Liu, Y.-P. 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Energy Storage. \u003cb\u003e134\u003c/b\u003e, 118203 (2025). \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttp://dx.doi.org/10.1016/j.est.2025.118203\u003c/span\u003e\u003cspan address=\"10.1016/j.est.2025.118203\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":true,"highlight":"","institution":"","isAcceptedByJournal":false,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true},"keywords":"Antiferroelectric, Energy storage performances, Dual-phase composite ceramics, Y2O3, Breakdown strength","lastPublishedDoi":"10.21203/rs.3.rs-9095268/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-9095268/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eAntiferroelectric (AFE) ceramics hold great promise for high energy density capacitors, though their energy storage properties (ESPs) are fundamentally limited by a relatively low breakdown electric field (\u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e). Hence, the dual-phase composite ceramics were designed by incorporating a pyrochlore phase into the perovskite matrix to enhance ESPs. Composite ceramics of Y\u003csub\u003e2\u003c/sub\u003eZr\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e7\u003c/sub\u003e modified Pb\u003csub\u003e0.94\u003c/sub\u003eLa\u003csub\u003e0.04\u003c/sub\u003eZr\u003csub\u003e0.99\u003c/sub\u003eTi\u003csub\u003e0.01\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e- \u003cem\u003ex\u003c/em\u003e wt% Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e were fabricated and investigated. The introduction of Y\u003csub\u003e2\u003c/sub\u003eZr\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e7\u003c/sub\u003e serves to reduce the overall dielectric permittivity (\u003cem\u003eε\u003c/em\u003e\u003csub\u003er\u003c/sub\u003e) and enhance insulation, which collectively raise the \u003cem\u003eE\u003c/em\u003e\u003csub\u003eb\u003c/sub\u003e from 420 kV/cm to 850 kV/cm. A maximum recoverable energy density (\u003cem\u003eW\u003c/em\u003e\u003csub\u003erec\u003c/sub\u003e) of 14.5 J/cm\u003csup\u003e3\u003c/sup\u003e with an energy efficiency (\u003cem\u003eη\u003c/em\u003e) of 85.7% are achieved in the ceramic with \u003cem\u003ex\u003c/em\u003e\u0026thinsp;=\u0026thinsp;4 under 570 kV/cm. In addition, a current density (\u003cem\u003eC\u003c/em\u003e\u003csub\u003eD\u003c/sub\u003e) as high as 2369.4 A/cm\u003csup\u003e2\u003c/sup\u003e, a power density (\u003cem\u003eP\u003c/em\u003e\u003csub\u003eD\u003c/sub\u003e) of 462 MW/cm\u003csup\u003e3\u003c/sup\u003e, and an ultrafast discharge rate of 22.6 ns are achieved. This work establishes the construction of dual-phase composites as a viable and novel approach to improving ESPs in PbZrO\u003csub\u003e3\u003c/sub\u003e (PZ) -based ceramic systems.\u003c/p\u003e","manuscriptTitle":"Ultrahigh energy storage performance in Pb0.94La0.04Zr0.99Ti0.01O3 ceramics via introducing pyrochlore phase Y2Zr2O7","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2026-04-20 17:46:59","doi":"10.21203/rs.3.rs-9095268/v1","editorialEvents":[{"type":"communityComments","content":0}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true}}],"origin":"","ownerIdentity":"552707d2-4109-4248-ace5-f6931608739b","owner":[],"postedDate":"April 20th, 2026","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"posted","subjectAreas":[],"tags":[],"updatedAt":"2026-05-16T12:54:28+00:00","versionOfRecord":[],"versionCreatedAt":"2026-04-20 17:46:59","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-9095268","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-9095268","identity":"rs-9095268","version":["v1"]},"buildId":"XKTyCvWXoU3ODBz1xrDgd","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}