Boosting Energy-Storage in High-Entropy Pb-Free Relaxors Engineered by Local Lattice Distortion

Banghua Zhu; Ji Zhang; Feixiang Long; Jue Liu; Andrea Sanson; Luca Olivi; Joerg C. Neuefeind; Hui Liu; Jun Chen

doi:10.1021/jacs.4c10907

Boosting Energy-Storage in High-Entropy Pb-Free Relaxors Engineered by Local Lattice Distortion

Banghua Zhu, Ji Zhang, Feixiang Long, Jue Liu, Andrea Sanson, Luca Olivi, Joerg C. Neuefeind, Hui Liu, Jun Chen

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Abstract

The high-entropy strategy has shown potential in advancing the energy-storage performance of dielectric capacitors, offering benefits to a range of electronic and electrical systems. However, designing high-performance high-entropy relaxor ferroelectrics (RFEs) presents challenges due to the unclear correlation between their core effects and local polarization heterogeneity. Here, we demonstrate that by engineering the local lattice distortion, a core effect in high-entropy systems, to manipulate the local polarization configuration, a giant energy density (W_rec) of 18.7 J cm^-3 and high efficiency (η) of 85% can be achieved in (Bi_0.5K_0.5)TiO₃-based high-entropy bulk RFE ceramics. Atomic-level local structural analysis unveils that the local lattice distortion field can be flattened by introducing ions with less size mismatch. The increase in configurational entropy from 1.54 to 2.06R is associated with a smoother polar displacement vector field and a reduction in the size of polar clusters to several unit-cell sizes with weak coupling. Consequently, a substantial decrease in hysteresis and an enhancement in the breakdown field strength can be obtained, leading to a significant improvement in energy density by over 6 times and efficiency by 3 times. Our research establishes a relationship between local lattice distortion, atomic polar displacement, and energy-storage performance in complex high-entropy systems, providing insights for enhancing energy-storage performance via a local structure design.

Original language	English
Pages (from-to)	29694-29702
Number of pages	9
Journal	Journal of the American Chemical Society
Volume	146
Issue number	43
DOIs	https://doi.org/10.1021/jacs.4c10907
State	Published - Oct 30 2024

Funding

This work was supported by the Key Research and Development Program of the Ministry of Science and Technology of China (No. 2022YFB3204000), the Outstanding Young Scientists Program of Beijing Higher Education Institutions (JWZQ20240101015), and the National Natural Science Foundation of China (Nos. 22235002 and 22075014). A portion of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. We acknowledge ELETTRA Sincrotrone Trieste for providing access to its synchrotron radiation facilities (spectra collected during Exp. 20230135) and all the staff of XAFS Beamline for technical assistance.

Funders	Funder number
Office of Science
Outstanding Young Scientists Program of Beijing Higher Education Institutions	JWZQ20240101015
National Natural Science Foundation of China	22235002, 22075014
Ministry of Science and Technology of the People's Republic of China	2022YFB3204000
Oak Ridge National Laboratory	20230135

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title = "Boosting Energy-Storage in High-Entropy Pb-Free Relaxors Engineered by Local Lattice Distortion",

abstract = "The high-entropy strategy has shown potential in advancing the energy-storage performance of dielectric capacitors, offering benefits to a range of electronic and electrical systems. However, designing high-performance high-entropy relaxor ferroelectrics (RFEs) presents challenges due to the unclear correlation between their core effects and local polarization heterogeneity. Here, we demonstrate that by engineering the local lattice distortion, a core effect in high-entropy systems, to manipulate the local polarization configuration, a giant energy density (Wrec) of 18.7 J cm-3 and high efficiency (η) of 85% can be achieved in (Bi0.5K0.5)TiO3-based high-entropy bulk RFE ceramics. Atomic-level local structural analysis unveils that the local lattice distortion field can be flattened by introducing ions with less size mismatch. The increase in configurational entropy from 1.54 to 2.06R is associated with a smoother polar displacement vector field and a reduction in the size of polar clusters to several unit-cell sizes with weak coupling. Consequently, a substantial decrease in hysteresis and an enhancement in the breakdown field strength can be obtained, leading to a significant improvement in energy density by over 6 times and efficiency by 3 times. Our research establishes a relationship between local lattice distortion, atomic polar displacement, and energy-storage performance in complex high-entropy systems, providing insights for enhancing energy-storage performance via a local structure design.",

author = "Banghua Zhu and Ji Zhang and Feixiang Long and Jue Liu and Andrea Sanson and Luca Olivi and Neuefeind, {Joerg C.} and Hui Liu and Jun Chen",

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AU - Sanson, Andrea

AU - Olivi, Luca

AU - Neuefeind, Joerg C.

AU - Liu, Hui

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AB - The high-entropy strategy has shown potential in advancing the energy-storage performance of dielectric capacitors, offering benefits to a range of electronic and electrical systems. However, designing high-performance high-entropy relaxor ferroelectrics (RFEs) presents challenges due to the unclear correlation between their core effects and local polarization heterogeneity. Here, we demonstrate that by engineering the local lattice distortion, a core effect in high-entropy systems, to manipulate the local polarization configuration, a giant energy density (Wrec) of 18.7 J cm-3 and high efficiency (η) of 85% can be achieved in (Bi0.5K0.5)TiO3-based high-entropy bulk RFE ceramics. Atomic-level local structural analysis unveils that the local lattice distortion field can be flattened by introducing ions with less size mismatch. The increase in configurational entropy from 1.54 to 2.06R is associated with a smoother polar displacement vector field and a reduction in the size of polar clusters to several unit-cell sizes with weak coupling. Consequently, a substantial decrease in hysteresis and an enhancement in the breakdown field strength can be obtained, leading to a significant improvement in energy density by over 6 times and efficiency by 3 times. Our research establishes a relationship between local lattice distortion, atomic polar displacement, and energy-storage performance in complex high-entropy systems, providing insights for enhancing energy-storage performance via a local structure design.

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Boosting Energy-Storage in High-Entropy Pb-Free Relaxors Engineered by Local Lattice Distortion

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