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Effect of Al substitution and secondary CuO phase on dielectric response in microwave-processed CaCu3Ti4−xAlxO12 ceramics

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Abstract

High dielectric loss is a major drawback in CCTO-based electroceramics, and such high dielectric loss supports good microwave coupling for microwave synthesis of ceramics. Al substitution at Ti site and presence of moderate amount of secondary CuO intergranular melt-like phase can improve the dielectric properties of the ceramics. Therefore, microwave-assisted solid-state reaction was used to synthesize polycrystalline CaCu3Ti4−xAlxO12 (x = 0, 0.025, 0.05, 0.075, 0.1) ceramics. Lattice parameters and different amount of CuO phase were extracted from X-ray diffraction data via Rietveld refinement. Presence of grains with different morphology, and different kind of interfaces were confirmed through microstructure evolution. An approximate elemental analysis was revealed through selective area EDX. Variations in dielectric and impedance properties with frequency and temperature were investigated as an effect of Al3+ substitution at Ti4+ sites and appearance of secondary CuO phase. Maximum dielectric constant (εr) ~ 23,000 with ‘tan δ’ ~ 0.076 at 100 Hz has been observed for x = 0.05 ceramics at room temperature. Equivalent electrical circuits were proposed to understand the contributions arising from different electrically heterogeneous portions of CCTO-based ceramics. An elementary theoretical framework, based on different grains and interfaces (boundaries), has been proposed to understand the improved dielectric properties. Activation energies were calculated from imaginary part of impedance (Z″) and modulus (M″) functions and the values were in close agreement with activation energies associated to oxygen vacancies. In addition, defect chemistry has been discussed to understand the appearance of CuO phase as melt and the improvement of dielectric loss.

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Acknowledgements

The authors acknowledge the financial support of DRDO (Government of India) [Project No. ERIP/ER/1406037/M/01/1558. We would like to thank Prof. Santosh Kumar Sahoo of department of Metallurgy and Materials Engineering [NIT Rourkela, Odisha, 769008] for measurement at X-ray Diffraction.

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Authors and Affiliations

  1. Department of Physics and Astronomy, National Institute of Technology, Rourkela, Odisha, 769008, India

    Buddhadev Samanta & P. Kumar

  2. Department of Physics, Lingaya’s Vidyapeeth, Faridabad, Haryana, 121002, India

    Dipika Nanda

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  1. Buddhadev Samanta
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Contributions

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

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Correspondence to P. Kumar.

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Authors confirm that there is no conflict of interest regarding submission of research paper titled “Effect of Al substitution and secondary CuO phase on dielectric response in microwave-processed CaCu3Ti4−xAlxO12 ceramics” authored by Buddhadev Samanta, P. Kumar, and Dipika Nanda to your esteemed journal for consideration of publication. Previously, this article has not been published elsewhere and presently not under consideration elsewhere. If accepted, the article will not be published elsewhere in the same form, in any language, without the written consent of the publisher.

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Samanta, B., Kumar, P. & Nanda, D. Effect of Al substitution and secondary CuO phase on dielectric response in microwave-processed CaCu3Ti4−xAlxO12 ceramics. J Mater Sci: Mater Electron 33, 1425–1440 (2022). https://doi.org/10.1007/s10854-021-07596-6

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