Dielectric ceramics are crucial for high-temperature, pulse-power energy storage applications. However, the mutual restriction between the polarization and breakdown strength has been a significant challenge. Here, multiphase engineering controlled by the two-step sintering heating rate is adopted to simultaneously obtain a high polarization and breakdown strength in 0.8(0.95Bi0.5Na0.5TiO3-0.05SrZrO3)-0.2NaNbO3 (BNTSZNN) ceramic systems. The coexistence of tetragonal (T) and rhombohedral (R) phases benefits the temperature stability of BNTSZNN ceramics. Increasing the heating rate during sintering reduces the diffusion of SrZrO3 and NaNbO3 into Bi0.5Na0.5TiO3, which results in a high proportion of the R phase and a finer grain size. The overall polarization is enhanced by increasing the proportion of the high-polarization R phase, which is demonstrated using a first-principles method. Meanwhile, the finer grain size enhances the breakdown strength. Following this design philosophy, an ultrahigh Wdis of 5.55 J/cm3 and η above 85% is achieved in BNTSZNN ceramics as prepared with a fast heating rate of 60 °C/min given a simultaneously high polarization of 43 μC/cm2 and high breakdown strength of 350 kV/cm. Variations in the discharge energy density from room temperature to 160 °C are less than 10%. Additionally, such BNTSZNN ceramics exhibit an ultrafast discharge speed with τ0.9 at approximately 60 ns, which shows great potential in pulse-power system applications.
Keywords: energy storage; high breakdown strength; high polarization; multiphase engineering; temperature stability.