Role of mixed oxidant and controlled oxygen partial pressure heat treatment to regulate the dielectric properties and resistivity of SrTiO3-based CP ceramics

Abstract

Sr0.99La0.01TiO3 (SLT10) colossal permittivity (CP) ceramic materials were synthesized using solid phase method and secondary heat treated using mixed oxidant 35%Bi2O3–10%Al2O3–20%MgO–25%CuO–10%SiO2 oxidant. The heat treatment atmospheres were chosen as O2, air, and Ar to correspond to different oxygen partial pressures. The dielectric properties of the Sr0.99La0.01TiO3-Percolated (SLT10-P) ceramics were investigated, and the contribution of the oxidant to the resistivity enhancement was verified by complex impedance spectroscopy and DC resistivity tests. Excellent dielectric properties were obtained for SLT10-P Air ceramic sample (16543 for dielectric permittivity and 0.016 for loss tangent), and the resistivity was increased from 2.13 × 108 Ω cm (SLT10) to 1.23 × 1011 Ω cm (SLT10-P Air). The resistance degradation mechanism of SLT10-P ceramics and oxygen vacancy migration in the process of resistance degradation were studied by using resistance monitoring device and thermally stimulated depolarization currents (TSDC) test. The introduction of oxidant optimizes the temperature stability and resistivity of SLT10 ceramics, but it will lead to the decrease of dielectric permittivity. The atmosphere of heat treatment changed the concentration of oxygen vacancy in ceramics. When SLT10-P O2 was treated in O2 atmosphere, the concentration of oxygen vacancy in ceramics decreased, which led to the decrease of dielectric permittivity and the increase of grain boundary resistance. For SLT10-P Ar ceramic, more oxygen vacancies and free electrons are induced by low oxygen partial pressure heat treatment, which enhances the dipole effect of electron pinning defects and leads to colossal dielectric permittivity, but high concentration of oxygen vacancies will affect the resistance decline. In SLT10-P Air ceramic, the coexistence of colossal permittivity and low loss tangent and high resistance is realized.