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Incorporation of Pb into the Crystal Structure of Ba6−3xNd8+2xTi18O54 Solid Solution
Published online by Cambridge University Press: 31 January 2011
Abstract
Investigations of a substitutional mechanism of Pb incorporation into the crystal structure of Ba6−3xNd8+2xTi18O54 performed by x-ray diffraction analysis, scanning electron microscopy, and energy dispersive and wavelength dispersive x-ray spectroscopy revealed that Pb2+ substitutes for Ba2+ according to the formula (Ba1−zPbz)6−3xNd8+2xTi18O54. The solid solubility limit for 0.5 = x = 0.6 compositions was determined to be at 0.35 ≤ z < 0.4 (nominal composition) which, according to measurements of PbO loss occurring during the heat treatment, gives 0.30 ≤ z < 0.35 (analyses of matrix phase). Increasing the Pb2+ concentration in (Ba1−zPbz)4.5Nd9Ti18O54, results in tf decreasing from an initial positive value (80 ppm/K) to a negative value at the solid solubility limit (−25 ppm/K at z = 0.35). In the same concentration range the Q-value decreases from an initial 2000 to 1250 (z. = 0.35), measured at 4 GHz, while permittivity remains almost constant (k = 87 ± 1.5). After exceeding the solid solubility limit of Pb2+ in (Ba1−zPbz)4.5Nd9Ti18O54 the appearance of secondary phases (Nd4Ti9O24 and Pb-rich phase at grain boundaries) changes the trends of the microwave dielectric properties; permittivity decreases, Q-value remains almost constant, and Tf increases.
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