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Abstract

Lead-free antiferroelectric (AFE) materials exhibiting relaxor behavior have emerged as a research focus for enhancing energy storage performance. The Na0.82Gd0.06NbO3xMnO2 (0 ≤ x ≤ 5 mol%) ceramics prepared by the traditional solid-state method show an AFE R phase structure at room temperature, which was verified by Rietveld refinement and Raman spectroscopy. The doping of MnO2 significantly enhances the dielectric relaxation behavior and realizes the transformation from a nearly linear polarization hysteresis loop to a ferroelectric-like one. This observation may be ascribed to the formation of polar nanoregions, which stems from the chemical disorder induced by the incorporation of Mn ions into the Na0.82Gd0.06NbO3 matrix. Besides, the complex impedance tests reveal the enhanced electrical homogeneity and densification in the MnO2-doped samples. The combined effect of grains and grain boundaries is responsible for the electrical conductivity in the MnO2-doped samples. The calculated activation energies for grains and grain boundaries explain the MnO2-concentration-dependent migration of oxygen vacancies within the grains and the grain boundaries during the conduction process. The tunable relaxor-like behavior and the linear polarization hysteresis loop observed in Na0.82Gd0.06NbO3xMnO2 (0 ≤ x ≤ 5 mol%) ceramics suggest their potential application in energy storage.

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Funding

This work was supported by the National Natural Science Foundation of China [Grant Number 11904304], Natural Science Foundation of Fujian Province [Grant Numbers 2021J011218 and 2021J011215] and Graduate Education Reform Project of Fujian University Alliance of Physics Discipline [Grant Number FJPHYS-2023-B09].

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Wenhao Xun: Conceptualization, Data curation, Formal analysis, Writing–original draft. Xiaohua Huang: Conceptualization, Resources, Validation, Supervision, Writing–review and editing. Zekun Li, Ying Hou, Jiajun Song, and Xue’e Xu: Investigation. Zaijun Cheng: Investigation, Resources.

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Xun, W., Huang, X., Li, Z. et al. Tailoring the relaxor-like behavior and electrical properties of Na0.82Gd0.06NbO3 ceramics via MnO2 doping. J Mater Sci: Mater Electron 36, 1226 (2025). https://doi.org/10.1007/s10854-025-15347-0

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