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BaTiO3 has advantages of high permittivity, low dielectric loss, low cost and environment friendly. However, due to the nonlinear dielectric behavior occurred around the phase transition temperature of BaTiO3 ceramic, its availability in the field of temperature-stable capacitor is limited. To modify the dielectric-temperature properties of BaTiO3, a series of BaTi1-xCexO3 (x=0-0.20) ceramics was synthesized by solid-state reaction method. Ce dopant was introduced into the B-site (Ti-site) of BaTiO3. The effects of Ce dopant on the phase evolution, defect state, microstructure and dielectric properties were investigated. The modifying mechanism was also discussed with the help of first-principles calculation method. In all ceramic samples, it is revealed that Ce element completely enters the B-site of BaTiO3 in the form of Ce4+ ion. With the increase of Ce doping concentration, the room temperature structure of BaTi1-xCexO3 ceramics transforms from tetragonal/pseudo-cubic structure into orthorhombic/tetragonal structure, then into pseudo-cubic structure. Owing to the radius difference between Ce4+ and Ti4+ ions, Ce doping will lead to the rising of lattice parameters, accompanied by the appearance of local distortion and the decrease of long-range ferroelectric order, the variation of band structure, density of states and charge density configuration, as well as the generation of Ba and Ti vacancies. Compared with pure BaTiO3 ceramic, the average grain size of Ce-doped ceramics decreases first and then increases with the increase of Ce content, while the relative density of ceramics increases gradually. The peak dielectric constant of BaTi1-xCexO3 ceramic increases first and then decreases as the Ce concentration increasing. The corresponding temperature is slowly reduced from 122 ℃ to 112 ℃ in the x value range of 0-0.08, then rapidly declines to -3 ℃ in the x value range of 0.08-0.20. BaTi1-xCexO3 ceramics with x≥0.06 have the dielectric behavior of diffused phase transition (DPT). And the x=0.20 ceramic exhibits the typical characteristic of relaxor ferroelectric, with the room temperature dielectric constant of 3258.38, and the |Δεr/εr25 ℃|≤22% temperature range of -60-87 ℃, which matches the requirement of EIA X5S standard. Therefore, it can be concluded that B-site Ce doping will effectively enhance the permittivity stability of BaTiO3 in a variable temperature environment. This will provide some new ideas to develop dielectric materials with stable dielectric properties in wide temperature range. |
