Synergistic Design Strategies Breaking the Energy Storage Trade-Off in Lead-Free Dielectrics

Ruiyi Jing; Leiyang Zhang; Yule Yang; Wanchang Man; Meng Meng; Yunyao Huang; Zibin Chen; Liqiang He; Nanxi Miao; He Qi; Bin Zhou; Xuefeng Chen; Hua Tan; Haibo Zhang; Jun Yang; Zupei Yang; Haibo Yang; Shujun Zhang; Li Jin

doi:10.1002/adma.74343

Synergistic Design Strategies Breaking the Energy Storage Trade-Off in Lead-Free Dielectrics

Ruiyi Jing
, Leiyang Zhang
, Yule Yang
, Wanchang Man
, Meng Meng
, Yunyao Huang
, Zibin Chen
, Liqiang He
, Nanxi Miao
, He Qi
, Bin Zhou
, Xuefeng Chen^*
, Hua Tan^*
, Haibo Zhang
, Jun Yang
, Zupei Yang
, Haibo Yang^*
, Shujun Zhang^*
, Li Jin^*

^*Corresponding author for this work

Department of Chemistry

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

1 Citation (Scopus)

Abstract

Development of lead-free dielectric capacitors with simultaneously high recoverable energy-storage (ES) density (W_rec) and breakdown strength (E_b) is hindered by a fundamental constraint; although high E_b permits large electric fields, conventional ferroelectrics suffer from premature polarization saturation, limiting further enhancement of W_rec. We demonstrate a mechanism-guided strategy for Bi_0.5Na_0.5TiO₃ (BNT)-based relaxor ferroelectric ceramics, centered on optimized polar nanoregion (PNR) responses and delayed polarization saturation. Phase-field simulations show that interconnected rhombohedral/tetragonal (R/T)-related PNRs with appropriate size and dynamic responsiveness can be progressively activated under electric fields, enabling delayed polarization saturation, sustained ΔP growth, and low hysteresis loss. Guided by this mechanism, compositional disorder, R/T phase coexistence are integrated in the BNT-based system to construct an optimized PNR landscape. The optimized multilayer ceramic capacitors deliver a record ES potential (ξ = W_rec/E_b) of 278 J kV⁻¹ m⁻², together with a high W_rec of 26.4 J cm⁻³ at 950 kV cm⁻¹ and 89% ES efficiency. Atomic-resolution microscopy confirms pronounced local chemical heterogeneity and coexisting R/T-related PNRs, consistent with the optimized PNR response predicted by phase-field simulations. These results establish a generalizable framework for overcoming the intrinsic ξ–E_b trade-off and advancing next-generation high-W_rec dielectric capacitors for ES and pulsed-power applications. © 2026 Wiley-VCH GmbH.

Original language	English
Article number	e74343
Number of pages	12
Journal	Advanced Materials
Online published	25 Jul 2026
DOIs	https://doi.org/10.1002/adma.74343
Publication status	Online published - 25 Jul 2026

Funding

This paper is dedicated to the 130th anniversary of Xi'an Jiaotong University and the 70th anniversary of the Westward Academic Relocation. This work was supported by the National Natural Science Foundation of China (52261135548, 52302153, and 52402155), the China Postdoctoral Science Foundation (GZC20232075 and 2023M742767), the Shaanxi Province Postdoctoral Research Project (2023BSHTBZZ14), and the Guangdong Basic and Applied Basic Research Foundation (2024A1515140014). SEM measurements were performed at the International Center for Dielectric Research (ICDR), Xi'an Jiaotong University, Xi'an, China.

Research Keywords

BNT-based ceramics
breakdown strength
energy storage capacitors
lead-free dielectrics
polar nanoregions
relaxor ferroelectrics

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Jing, R., Zhang, L., Yang, Y., Man, W., Meng, M., Huang, Y., Chen, Z., He, L., Miao, N., Qi, H., Zhou, B., Chen, X., Tan, H., Zhang, H., Yang, J., Yang, Z., Yang, H., Zhang, S., & Jin, L. (2026). Synergistic Design Strategies Breaking the Energy Storage Trade-Off in Lead-Free Dielectrics. Advanced Materials, Article e74343. Advance online publication. https://doi.org/10.1002/adma.74343

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title = "Synergistic Design Strategies Breaking the Energy Storage Trade-Off in Lead-Free Dielectrics",

abstract = "Development of lead-free dielectric capacitors with simultaneously high recoverable energy-storage (ES) density (Wrec) and breakdown strength (Eb) is hindered by a fundamental constraint; although high Eb permits large electric fields, conventional ferroelectrics suffer from premature polarization saturation, limiting further enhancement of Wrec. We demonstrate a mechanism-guided strategy for Bi0.5Na0.5TiO3 (BNT)-based relaxor ferroelectric ceramics, centered on optimized polar nanoregion (PNR) responses and delayed polarization saturation. Phase-field simulations show that interconnected rhombohedral/tetragonal (R/T)-related PNRs with appropriate size and dynamic responsiveness can be progressively activated under electric fields, enabling delayed polarization saturation, sustained ΔP growth, and low hysteresis loss. Guided by this mechanism, compositional disorder, R/T phase coexistence are integrated in the BNT-based system to construct an optimized PNR landscape. The optimized multilayer ceramic capacitors deliver a record ES potential (ξ = Wrec/Eb) of 278 J kV−1 m−2, together with a high Wrec of 26.4 J cm−3 at 950 kV cm−1 and 89\% ES efficiency. Atomic-resolution microscopy confirms pronounced local chemical heterogeneity and coexisting R/T-related PNRs, consistent with the optimized PNR response predicted by phase-field simulations. These results establish a generalizable framework for overcoming the intrinsic ξ–Eb trade-off and advancing next-generation high-Wrec dielectric capacitors for ES and pulsed-power applications. {\textcopyright} 2026 Wiley-VCH GmbH.",

keywords = "BNT-based ceramics, breakdown strength, energy storage capacitors, lead-free dielectrics, polar nanoregions, relaxor ferroelectrics",

author = "Ruiyi Jing and Leiyang Zhang and Yule Yang and Wanchang Man and Meng Meng and Yunyao Huang and Zibin Chen and Liqiang He and Nanxi Miao and He Qi and Bin Zhou and Xuefeng Chen and Hua Tan and Haibo Zhang and Jun Yang and Zupei Yang and Haibo Yang and Shujun Zhang and Li Jin",

year = "2026",

month = jul,

day = "25",

doi = "10.1002/adma.74343",

language = "English",

journal = "Advanced Materials",

issn = "0935-9648",

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TY - JOUR

T1 - Synergistic Design Strategies Breaking the Energy Storage Trade-Off in Lead-Free Dielectrics

AU - Jing, Ruiyi

AU - Zhang, Leiyang

AU - Yang, Yule

AU - Man, Wanchang

AU - Meng, Meng

AU - Huang, Yunyao

AU - Chen, Zibin

AU - He, Liqiang

AU - Miao, Nanxi

AU - Qi, He

AU - Zhou, Bin

AU - Chen, Xuefeng

AU - Tan, Hua

AU - Zhang, Haibo

AU - Yang, Jun

AU - Yang, Zupei

AU - Yang, Haibo

AU - Zhang, Shujun

AU - Jin, Li

PY - 2026/7/25

Y1 - 2026/7/25

N2 - Development of lead-free dielectric capacitors with simultaneously high recoverable energy-storage (ES) density (Wrec) and breakdown strength (Eb) is hindered by a fundamental constraint; although high Eb permits large electric fields, conventional ferroelectrics suffer from premature polarization saturation, limiting further enhancement of Wrec. We demonstrate a mechanism-guided strategy for Bi0.5Na0.5TiO3 (BNT)-based relaxor ferroelectric ceramics, centered on optimized polar nanoregion (PNR) responses and delayed polarization saturation. Phase-field simulations show that interconnected rhombohedral/tetragonal (R/T)-related PNRs with appropriate size and dynamic responsiveness can be progressively activated under electric fields, enabling delayed polarization saturation, sustained ΔP growth, and low hysteresis loss. Guided by this mechanism, compositional disorder, R/T phase coexistence are integrated in the BNT-based system to construct an optimized PNR landscape. The optimized multilayer ceramic capacitors deliver a record ES potential (ξ = Wrec/Eb) of 278 J kV−1 m−2, together with a high Wrec of 26.4 J cm−3 at 950 kV cm−1 and 89% ES efficiency. Atomic-resolution microscopy confirms pronounced local chemical heterogeneity and coexisting R/T-related PNRs, consistent with the optimized PNR response predicted by phase-field simulations. These results establish a generalizable framework for overcoming the intrinsic ξ–Eb trade-off and advancing next-generation high-Wrec dielectric capacitors for ES and pulsed-power applications. © 2026 Wiley-VCH GmbH.

AB - Development of lead-free dielectric capacitors with simultaneously high recoverable energy-storage (ES) density (Wrec) and breakdown strength (Eb) is hindered by a fundamental constraint; although high Eb permits large electric fields, conventional ferroelectrics suffer from premature polarization saturation, limiting further enhancement of Wrec. We demonstrate a mechanism-guided strategy for Bi0.5Na0.5TiO3 (BNT)-based relaxor ferroelectric ceramics, centered on optimized polar nanoregion (PNR) responses and delayed polarization saturation. Phase-field simulations show that interconnected rhombohedral/tetragonal (R/T)-related PNRs with appropriate size and dynamic responsiveness can be progressively activated under electric fields, enabling delayed polarization saturation, sustained ΔP growth, and low hysteresis loss. Guided by this mechanism, compositional disorder, R/T phase coexistence are integrated in the BNT-based system to construct an optimized PNR landscape. The optimized multilayer ceramic capacitors deliver a record ES potential (ξ = Wrec/Eb) of 278 J kV−1 m−2, together with a high Wrec of 26.4 J cm−3 at 950 kV cm−1 and 89% ES efficiency. Atomic-resolution microscopy confirms pronounced local chemical heterogeneity and coexisting R/T-related PNRs, consistent with the optimized PNR response predicted by phase-field simulations. These results establish a generalizable framework for overcoming the intrinsic ξ–Eb trade-off and advancing next-generation high-Wrec dielectric capacitors for ES and pulsed-power applications. © 2026 Wiley-VCH GmbH.

KW - BNT-based ceramics

KW - breakdown strength

KW - energy storage capacitors

KW - lead-free dielectrics

KW - polar nanoregions

KW - relaxor ferroelectrics

UR - https://www.scopus.com/pages/publications/105045670546

UR - https://www.scopus.com/pages/publications/105045670546#tab=impact

U2 - 10.1002/adma.74343

DO - 10.1002/adma.74343

M3 - RGC 21 - Publication in refereed journal

SN - 0935-9648

JO - Advanced Materials

JF - Advanced Materials

M1 - e74343

ER -

Synergistic Design Strategies Breaking the Energy Storage Trade-Off in Lead-Free Dielectrics

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Research Keywords

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