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Oxygen-vacancy-related dielectric relaxations and electrical properties in [Lix(BaSrCaMg)(1−x)/4]TiO3 high-entropy perovskite ceramics

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Abstract

High-entropy perovskite ceramics, [Lix(BaSrCaMg)(1−x)/4]TiO3 (x = 0.1, 0.15, 0.2, 0.3), were designed and successfully synthesized by solid-state method. The effects of Li contents on the phase formation, microstructures, and the origin of dielectric relaxation of all ceramics have been systematically investigated. The results show that all ceramics exhibit perovskite structure, and increasing Li content is conducive to grain growth and the formation of dense ceramics. XPS and EPR prove that oxygen vacancies increase with the increase of Li content. It is observed at room temperature that the increase of Li content not only contributes to the improved permittivity but also results in high-dielectric loss. Two sets of dielectric relaxations are observed in all ceramics. The lower temperature relaxation is shown to originate from the interfacial polarization, while the higher temperature relaxation is ascribed to double-ionized oxygen vacancies. The rapid increase of permittivity at higher temperatures and lower frequencies can be explained by space charge related to oxygen vacancies.

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Data availability

We confirm that material described in the manuscript, including all relevant raw data, will be freely available to any researcher wishing to use them for non-commercial purposes, without breaching participant confidentiality. The datasets generated during and/or analysed during the current study are available from the corresponding author on reasonable request.

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Acknowledgements

This work was supported by National Natural Science Foundation of China under Grant (No. 51972048).

Funding

Funding was provided by National Natural Science Foundation of China (Grant Number 51972048).

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Authors and Affiliations

  1. School of Materials Science and Engineering, Northeastern University, Shenyang, 110189, China

    Jun Zhang, Haowen Liu, Yaohang Gu, Jinrong Zhang & Xiaoyan Zhang

  2. College of Metallurgy and Energy, North China of Science and Technology, Tangshan, 063210, China

    Xiwei Qi

  3. School of Resources and Materials, Northeastern University at Qinhuangdao, Qinhuangdao, 066004, China

    Xiaoyan Zhang

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  1. Jun Zhang
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Contributions

All authors contributed to the study conception and design. Material preparation, data collection and analysis were performed by JZ, the first draft of the manuscript was written by JZ and all authors commented on previous versions of the manuscript. All authors read and approved the final manuscript.

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Correspondence to Xiwei Qi.

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We would like to declare on behalf of my co-authors that the work described is original research and has not been published previously, and not under consideration for publication elsewhere, in whole or in part. All the authors listed have approved the manuscript that is enclosed, and there is no conflict of interests during the submission of this manuscript. If accepted, this manuscript will not be published elsewhere in the same form, in English or in any other language, without the written consent.

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Zhang, J., Liu, H., Gu, Y. et al. Oxygen-vacancy-related dielectric relaxations and electrical properties in [Lix(BaSrCaMg)(1−x)/4]TiO3 high-entropy perovskite ceramics. J Mater Sci: Mater Electron 33, 9918–9929 (2022). https://doi.org/10.1007/s10854-022-07982-8

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