Abstract
Dielectric capacitors are critical for advanced energy storage due to their ultrahigh power density and rapid charge-discharge rates. However, their application is limited by the low energy density. Here, we design a BaTiO3-(K0.5Na0.5)NbO3-(Bi0.5Na0.5)Ti0.9Zr0.1O3 solid-solution system through synergistic polymorphic nanodomain engineering and defect optimization. By engineering polymorphic nanodomains with coexisting rhombohedral, orthorhombic, tetragonal, cubic nanodomain in 1.0–2.0 nm size and defect design with reduces oxygen vacancy concentration and forms defect complexes, we achieve an ultrahigh energy density of 18.7 J cm⁻3 with remarkable efficiency of 92.1% in multilayer ceramic capacitors, along with excellent cycling stability (>107 cycles) and thermal stability (<±5% from 25 to 150 °C). In this work, we provide a paradigm for designing high-performance dielectric capacitors through the synergistic manipulation of domain structures and defect engineering.
Similar content being viewed by others
Data availability
The data supporting the findings of this study are available in the paper and its Supplementary Information. The source data used in this study have been deposited in the Figshare database.
References
Chu, B. et al. A dielectric polymer with high electric energy density and fast discharge speed. Science 313, 334–336 (2006).
Pan, H. et al. Ultrahigh–energy density lead-free dielectric films via polymorphic nanodomain design. Science 365, 578–582 (2019).
Kim, J. et al. Ultrahigh capacitive energy density in ion-bombarded relaxor ferroelectric films. Science 369, 81–84 (2020).
Zhang, M. et al. Ultrahigh energy storage in high-entropy ceramic capacitors with polymorphic relaxor phase. Science 384, 185–189 (2024).
Li, J. et al. Grain-orientation-engineered multilayer ceramic capacitors for energy storage applications. Nat. Mater. 19, 999–1005 (2020).
Yang, B. et al. High-entropy enhanced capacitive energy storage. Nat. Mater. 21, 1074–1080 (2022).
Li, Y. et al. Enhanced energy storage performance in NBT-based MLCCs via cooperative optimization of polarization and grain alignment. Nat. Commun. 15, 8958 (2024).
Yang, L. et al. Perovskite lead-free dielectrics for energy storage applications. Prog. Mater. Sci. 102, 72–108 (2019).
Yang, B. et al. Balancing polarization and breakdown for high capacitive energy storage by microstructure design. Adv. Mater. 36, 2403400 (2024).
Zhu, L. F. et al. Boosting energy storage performance of BiFeO3-based multilayer capacitors via enhancing ionic bonding and relaxor behavior. J. Mater. Chem. A 10, 7382–7390 (2022).
Zhou, Z. et al. Ultrahigh capacitive energy storage of BiFeO3-based ceramics through multi-oriented nanodomain construction. Nat. Commun. 16, 2075 (2025).
Gao, P. et al. Enhanced energy-storage properties in (Bi0.5Na0.5)TiO3 ceramics by doping linear perovskite materials Ca0.85Bi0.1(Sn0.5Ti0.5)O3. Chem. Eng. J. 488, 151070 (2024).
Wei, T. et al. High-entropy assisted capacitive energy storage in relaxor ferroelectrics by chemical short-range order. Nat. Commun. 16, 807 (2025).
Pan, H. et al. Giant energy density and high efficiency achieved in bismuth ferrite-based film capacitors via domain engineering. Nat. Commun. 9, 1813 (2018).
Fu, J. et al. A highly polarizable concentrated dipole glass for ultrahigh energy storage. Nat. Commun. 15, 7338 (2024).
Chen, L. et al. Giant energy-storage density with ultrahigh efficiency in lead-free relaxors via high-entropy design. Nat. Commun. 13, 3089 (2022).
Li, W. et al. Generative learning facilitated discovery of high-entropy ceramic dielectrics for capacitive energy storage. Nat. Commun. 15, 4940 (2024).
Liu, H. et al. Chemical design of Pb-free relaxors for giant capacitive energy storage. J. Am. Chem. Soc. 145, 11764–11772 (2023).
Zheng, H. et al. 1-x) SBKT-xLMT lead-free ceramics with exceptional temperature stability and high energy density. Chem. Eng. J. 512, 162493 (2025).
Zheng, Q. et al. Ultrahigh breakdown strength of NaNbO3-based dielectric ceramics for high-voltage capacitor application. J. Am. Ceram. Soc. 107, 5490–5501 (2024).
Huang, Y. N. et al. Enhanced energy storage performances in A-/B-site modified BiFeO3-based relaxor ferroelectric ceramics. J. Am. Ceram. Soc. e20657 (2025).
Yan, F. et al. Significantly enhanced energy storage density and efficiency of BNT-based perovskite ceramics via A-site defect engineering. Energy Storage Mater. 30, 392–400 (2020).
Alkathy, M. S. et al. Achieving high energy storage density simultaneously with large efficiency and excellent thermal stability by defect dipole, and microstructural engineering in modified-BaTiO3 ceramics. J. Alloy. Compd. 934, 167887 (2023).
Li, P. et al. Local defect structure design enhanced energy storage performance in lead-free antiferroelectric ceramics. Chem. Eng. J. 497, 154926 (2024).
Shi, D. et al. Achieving ultrahigh energy storage density and efficiency above 90% via reducing defect concentrations for AgNbO3-based multilayer capacitors. Chem. Eng. J. 479, 147672 (2024).
Zhang, Z. et al. Defect engineering design and electrical breakdown model improve dielectric properties and reliability of rare-earth doped BaTiO3-based ceramics. Ceram. Int. 51, 705–715 (2025).
Pan, H. et al. Enhanced electric resistivity and dielectric energy storage by vacancy defect complex. Energy Storage Mater. 42, 836–844 (2021).
Zeng, X. et al. Polymorphic relaxor phase and defect dipole polarization co-reinforced capacitor energy storage in temperature-monitorable high-entropy ferroelectrics. Nat. Commun. 16, 1870 (2025).
Yang, Y. et al. Morphotropic relaxor boundary in a relaxor system showing enhancement of electrostrain and dielectric permittivity. Phys. Rev. Lett. 123, 137601 (2019).
Yang, G. et al. Distilling nanoscale heterogeneity of amorphous silicon using tip-enhanced Raman spectroscopy (TERS) via multiresolution manifold learning. Nat. Commun. 12, 578 (2021).
Shannon, R. D. Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides. Acta Cryst. 32, 751–767 (1976).
Zha, J. et al. High energy storage performance of KNN-based relaxor ferroelectrics in multiphase-coexisted superparaelectric state. J. Appl. Phys. 136, 074101 (2024).
Chen, I. Theory of thermally stimulated current in hopping systems. J. Appl. Phys. 47, 2988–2994 (1976).
Liu, W. & Randall, C. A. Thermally stimulated relaxation in Fe-doped SrTiO3 systems: I. Single crystals. J. Am. Ceram. Soc. 91, 3245–3250 (2008).
Liu, W. & Randall, C. A. Thermally stimulated relaxation in Fe-doped SrTiO3 systems: II. Degradation of SrTiO3 dielectrics. J. Am. Ceram. Soc. 91, 3251–3257 (2008).
Zhang, J. et al. Microwave dielectric properties and thermally stimulated depolarization currents of MgF2-doped diopside ceramics. J. Am. Ceram. Soc. 97, 3537–3543 (2014).
Guo, W. et al. Structure, defects, and microwave dielectric properties of Al-doped and Al/Nd co-doped Ba4Nd9.33Ti18O54 ceramics. J. Adv. Ceram. 11, 629–640 (2022).
Song, H. et al. Review of the thermally stimulated depolarization current (TSDC) technique for characterizing dielectric materials. J. Korean Ceram. Soc. 60, 747–759 (2023).
Zhang, J. et al. Understanding the thermally stimulated relaxation and defect behavior of Ti-containing microwave dielectrics: a case study of BaTi4O9. Mater. Des. 130, 479–487 (2017).
Guo, W. et al. Lattice dynamics and terahertz response of microwave dielectrics: a case study of Al-doped Ca0.6Sm0.27TiO3 ceramics. J. Eur. Ceram. Soc. 42, 4953–4961 (2022).
Guo, W. et al. Defect-related broadband dielectric loss mechanisms of Na1/2Sm1/2Ti1–z(Al1/2Nb1/2)zO3 ceramics. Acta Mater. 255, 119093 (2023).
Guo, W. et al. Microwave dielectric properties and thermally stimulated depolarization of Al-doped Ba4(Sm, Nd)9.33Ti18O54 ceramics. J. Am. Ceram. Soc. 102, 5494–5502 (2019).
Tang, T. et al. Self-generated glass-ceramics-like structure boosts energy storage performance of AgNbO3-based MLCC. Adv. Funct. Mater. 35, 2425711 (2025).
Li, J. et al. Enhanced energy-storage in lead-free multilayer capacitors via entropy-assisted polymorphic domain engineering. Nat. Commun. 16, 8580 (2025).
Zhu, L. F. et al. Heterovalent-doping-enabled atom-displacement fluctuation leads to ultrahigh energy-storage density in AgNbO3-based multilayer capacitors. Nat. Commun. 14, 1166 (2023).
Zhang, L. et al. Ultra-weak polarization-strain coupling effect boosts capacitive energy storage. Adv. Mater. 36, 2406219 (2024).
Li, J., Li, F., Xu, Z. & Zhang, S. Antiferroelectrics: Multilayer Lead-Free Ceramic Capacitors with Ultrahigh Energy Density and Efficiency. Adv. Mater. 30, 1870240 (2018).
Zheng, B. et al. High entropy-driven large capacitive energy storage in BaTiO3-based multilayer ceramic capacitors. Adv. Energy Mater. e04126 (2025).
Montecillo, R. et al. Ultrahigh energy storage in multilayer BiFeO3–BaTiO3–NaTaO3 relaxor ferroelectric ceramics. J. Mater. Chem. A 12, 30642–30654 (2024).
Lv, Z. et al. NaNbO3-based multilayer ceramic capacitors with ultrahigh energy storage performance. Adv. Energy Mater. 14, 2304291 (2024).
Yang, Y. et al. Giant energy storage density with ultrahigh efficiency in multilayer ceramic capacitors via interlaminar strain engineering. Nat. Commun. 16, 1300 (2025).
Xie, A. et al. Superior capacitive energy storage of NaNbO3-based MLCCs enabled by heterogeneous short-range ferroic orders. Adv. Funct. Mater. e16297 (2025).
Zhao, P. et al. Ultra-high energy storage performance in lead-free multilayer ceramic capacitors via a multiscale optimization strategy. Energy Environ. Sci. 13, 4882–4890 (2020).
Glaum, J. & Hoffman, M. Electric fatigue of lead-free piezoelectric materials. J. Am. Ceram. Soc. 97, 665–680 (2014).
Shvartsman, V. V. & Lupascu, D. C. Lead-free relaxor ferroelectrics. J. Am. Ceram. Soc. 95, 1–26 (2012).
Acknowledgements
This work was financially supported by the Basic Science Center Project of the National Natural Science Foundation of China (NSFC) (grant number 52388201); the National Key Research Program of China (grant numbers 2021YFB3800601); the NSFC (grant numbers 12574100, 52502143); Taishan Scholar Foundation of Shandong Province (tsqn202507050); Natural Science Foundation of Shandong Province (ZR2025QC473); Basic Research Program of Jiangsu (BK20250430); Guangdong Basic and Applied Basic Research Foundation (2024A1515110042); Shenzhen Science and Technology Program (Grant No. JCYJ20250604175816022), State Key Laboratory of New Ceramic Materials Tsinghua University (Nos. KF202408, KF202502); Young Talent of Lifting engineering for Science and Technology in Shandong, China (SDAST2024QTA056); and the Qilu Young Scholar Program of Shandong University.
Author information
Authors and Affiliations
Contributions
Y.-H.L. and M.Z. conceived this study. M.Z. and H.P. performed this study under the supervision of Y.-H.L. and C.-W.N. M.Z. and H.D.C. synthesized the samples and conducted out the electrical measurements. Q.H.Z. and Y.Z.H. conducted the STEM analysis. M.Z. and P.X.J. carried out the electrical measurements of the MLCCs. M.Z. and W.J.G. performed the TSDC measurement. M.Z. wrote the first draft of the manuscript. H.P., Y.-H.L., and C.-W.N. revised the paper. All authors discussed the results and revised the manuscript.
Corresponding author
Ethics declarations
Competing interests
The authors declare no competing interests.
Peer review
Peer review information
Nature Communications thanks Hangfeng Zhang and the other anonymous reviewer(s) for their contribution to the peer review of this work. A peer review file is available.
Additional information
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary information
Rights and permissions
Open Access This article is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License, which permits any non-commercial use, sharing, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if you modified the licensed material. You do not have permission under this licence to share adapted material derived from this article or parts of it. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by-nc-nd/4.0/.
About this article
Cite this article
Zhang, M., He, Y., Pan, H. et al. Ultrahigh energy-storage dielectric ceramics via synergistic polymorphic nanodomain and defect design. Nat Commun (2026). https://doi.org/10.1038/s41467-026-70768-7
Received:
Accepted:
Published:
DOI: https://doi.org/10.1038/s41467-026-70768-7


