Remarkable dielectric properties and enhanced hardness were achieved in high-entropy TiO2-based ceramics in this work by incorporating multiple pairs of donor-acceptor (D-A) cations (D = Nb5+, A = In3+, Al3+, Fe3+, Ga3+, La3+). The introduction of high-entropy engineering may facilitate the creation of favorable and stable microstructural features as lattice distorted and localized defect cluster, thereby enhancing the dielectric performance, thermal stability and mechanic properties. The composition of [Nb0.5(In0.2Al0.2Fe0.2Ga0.2La0.2)0.5]0.01Ti0.99O2 exhibits remarkably colossal permittivity (εr) value of approximately 18488 and low dielectric loss (tanδ) value of around 0.014 at 1 kHz. Furthermore, the thermal stability of the dielectric permittivity for [Nb0.5(In0.2Al0.2Fe0.2Ga0.2La0.2)0.5]0.01Ti0.99O2 ceramic meets the X9D standard, and the dielectric loss stays below ∼ 0.05 in the temperature range from -55 to 150 °C. Besides, the Vickers-hardness of [Nb0.5(In0.2Al0.2Fe0.2Ga0.2La0.2)0.5]0.01Ti0.99O2 gets increased by over 37% as compared to that of (Nb5+, In3+) co-doped ceramic (INTO). We presented in this work the influence of high-entropy on the dielectric and mechanic properties of TiO2-based ceramics, offering valuable insight into future development of colossal dielectric ceramics.
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