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Engineering relaxors by entropy for high energy storage performance

Nature Energy volume 8, pages 956–964 (2023)Cite this article

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Abstract

Relaxor ferroelectrics are the primary candidates for high-performance energy storage dielectric capacitors. A common approach to tuning the relaxor properties is to regulate the local compositional inhomogeneity, but there is a lack of a quantitative evaluation way for compositional fluctuation in relaxors. Here we propose configurational entropy as an index for the quantitative evaluation of local compositional inhomogeneity. Our results reveal that the local inhomogeneity increases with the entropy via scanning transmission electron microscopy, and relaxor features are accordingly modulated. With the deliberate design of entropy, we achieve an optimal overall energy storage performance in Bi4Ti3O12-based medium-entropy films, featuring a high energy density of 178.1 J cm−3 with efficiency exceeding 80% and a high figure of merit of 913. By using the medium-entropy films as dielectric layers, we demonstrate a multilayer film capacitor prototype that outperforms conventional multilayer ceramic capacitors.

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Fig. 1: Enhancing the relaxor properties and energy storage performance through entropy engineering.
Fig. 2: Phase structure and STEM-EDS analysis.
Fig. 3: Evolutions of local inhomogeneity and relaxor features by entropy modulation.
Fig. 4: Energy storage performances of the entropy-modulated films.

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Data availability

The data supporting the findings of this study are available within the paper and its Supplementary Information files. Source data are provided with this paper and are available at https://figshare.com/articles/dataset/SourceData_for_Engineering_the_relaxors_by_entropy_for_high_energy-storage_performance/23256506.

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Acknowledgements

We thank Z. Zhou and J. Qi for fruitful discussions. L.-Q.C. acknowledges the generous support by the Hamer Foundation through a Hamer Professorship at Penn State. This work was financially supported by the National Key Research Program of China (grant numbers 2021YFB3800601, Y.-H.L.); the Basic Science Center Project of the National Natural Science Foundation of China (NSFC) (grant number 52388201, Y.-H.L. and C.-W.N.); the Guangdong Basic and Applied Basic Research Foundation (2022A1515110048, B.Y.); the NSFC (grant numbers 52025025, 52072400 and 52103284, Q.Z., L.G and F.M.); the NSFC (grant number 51972028, H.H.).

Author information

Author notes

  1. These authors contributed equally: Bingbing Yang, Qinghua Zhang, Houbing Huang.

Authors and Affiliations

  1. State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, China

    Bingbing Yang, Fanqi Meng, Shun Lan, Yiqian Liu, Bin Wei, Yiqun Liu, Letao Yang, Ce-Wen Nan & Yuan-Hua Lin

  2. Foshan (Southern China) Institute for New Materials, Foshan, China

    Bingbing Yang

  3. Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, China

    Qinghua Zhang & Fanqi Meng

  4. Advanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing, China

    Houbing Huang & Wenxuan Zhu

  5. Department of Materials Science and Engineering, University of California, Berkeley, Berkeley, CA, USA

    Hao Pan

  6. National Center of Electron Microscopy in Beijing, School of Materials Science and Engineering, Tsinghua University, Beijing, China

    Lin Gu

  7. Department of Materials Science and Engineering Materials Research Institute, The Pennsylvania State University, University Park, PA, USA

    Long-Qing Chen

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Contributions

Y.-H.L. and B.Y. conceived this study. B.Y. performed this study with the supervision of Y.-H.L. C.-W.N. H.H., W.Z. and L.-Q.C. performed the phase-field simulations. B.W. performed the first-principles calculation. B.Y., S.L. and Yiqian Liu prepared the samples and measured the electrical properties. Q.Z., F.M. and L.G. performed the STEM characterizations. Yiqun Liu and L.Y. discussed the results. B.Y. wrote the first draft of the paper. H.P., Y.-H.L. and C.-W.N. revised the paper. All authors discussed the results and commented on the paper.

Corresponding authors

Correspondence to Ce-Wen Nan or Yuan-Hua Lin.

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Nature Energy thanks Lane Martin and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Extended data

Extended Data Fig. 1 Temperature dependent permittivity and loss tangent.

Temperature dependent permittivity and loss tangent of the films. a, x = 0.0. b, x = 0.4. c, x = 1.0. d, x = 1.5. e, x = 2.0 and f, x = 2.2.

Source data

Extended Data Fig. 2 Comparison of the Pm/Pr and Uloss.

Comparison of the Pm/Pr and Uloss of these entropy-modulated films at electric field of 2 MV cm−1.

Source data

Extended Data Fig. 3 Bipolar P-E loops.

Bipolar P-E loops at 10 kHz of these entropy-modulated films at electric field up to breakdown field. a, x = 0.0. b, x = 0.4. c, x = 1.0. d, x = 1.5. e, x = 2.0. f, x = 2.2.

Source data

Extended Data Fig. 4 The cross-section microstructure and breakdown property of the multilayer film capacitors.

a, Cross-sectional SEM image of the multilayer film capacitor. b and c, EDS-SEM images show the elemental distributions of Bi (b) and Au (c) elements, showing clear interfaces between dielectric layers and inner electrode layers. d, Weibull distribution analysis of the characteristic breakdown fields of the multilayer film capacitors.

Source data

Supplementary information

Supplementary Information

Supplementary Notes 1–4, Figs. 1–14, Tables 1–3 and References.

Source data

Source Data Fig. 1

Polarization, energy density, efficiency and figure of merit source data.

Source Data Fig. 2

XRD source data.

Source Data Fig. 3

Relaxor features, polarization and energy storage source data.

Source Data Fig. 4

Breakdown and energy storage source data.

Source Data Extended Data Fig. 1

Dielectric properties source data.

Source Data Extended Data Fig. 2

Polarization source data.

Source Data Extended Data Fig. 3

P–E loops source data.

Source Data Extended Data Fig. 4

Breakdown field source data.

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Yang, B., Zhang, Q., Huang, H. et al. Engineering relaxors by entropy for high energy storage performance. Nat Energy 8, 956–964 (2023). https://doi.org/10.1038/s41560-023-01300-0

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