Studies of structural and dielectric properties of lead-free perovskite K 0.5 Na 0.5 NbO 3 (KNN) ceramics obtained by the substitution of 5 at% of La and Ti for ions in the A-site and B-site, respectively, and sintered at different temperatures between 1100°C and 1190°C, are presented. X-ray diffraction patterns show the successful formation of an orthorhombic perovskite phase similar to that of pure KNN. The effect of doping and sintering temperature on the dielectric properties of the resulting ceramics is discussed. Simultaneous substitution of La and Ti into the KNN (KNNLaTi) causes a shift in the ferroelectricparaelectric phase transition temperature from that of pure KNN (420°C) to considerably lower ones (81 to 110°C) for the modified compounds. A particularly important result is the appearance of a single peak in the permittivity vs. temperature curve associated with the ferroelectric-paraelectric phase transition, where the KNNLaTi compound changes from orthorhombic to cubic structure, instead of the two reported for pure KNN. This transition exhibits the characteristics of a normal diffuse phase transition with an incipient relaxer behavior.
Pure K 0.5 Na 0.5 NbO 3 (KNN) and KNN doped with Li + (6% mole), La 3+ (1.66%, 5%, 6% mole), and Ti 4+ (10% mole) were prepared by mixture of oxides using high-energy milling and conventional solid-state reaction. The effects of the dopant on the physical properties of pure KNN have been evaluated based on the structural, ferroelectric, pyroelectric, and dielectric measurements. The XRD measurements show that KNN pure sample contains a mixture of monoclinic and orthorhombic crystalline phases, with a slightly higher concentration of monoclinic phase. In contrast, all doped samples show a higher concentration of the orthorhombic phase, as well as the presence of a secondary phase (K 6 Nb 10.8 O 30), also detected by Raman measurements. The samples with a higher concentration of this secondary phase, also present greater dielectric losses and lower values of remnant polarization. The dielectric measurements allowed us to detect temperatures of structural transitions (orthorhombic-tetragonal, O-T) previous to the ferroelectric-paraelectric transition (tetragonal-cubic, T-C), and also in this set of samples, a direct correlation was found between the values of remnant polarization and the corresponding pyroelectric signal response.
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