Enhancement of energy storage performance in lead‐free relaxor ferroelectric ceramics via band structure engineering

Abstract Dielectric capacitors with excellent energy storage performance (ESP) are in great demand in the power electronics industry due to their high power density. For the dielectric materials, the dielectric breakdown strength (BDS) is the key factor to improve ESP, which is the focus and bottleneck of current research, especially in the relaxor ferroelectric (RFE) materials with already low residual polarization (P r ). Here, we stimulate the ESP of the BaTiO 3 (BT)‐based RFE ceramics by band structure engineering. The Ta element is selected to enhance the band gap of doped ceramics, occupying Ti‐site in supercell of BT and optimizing the bonds length of Ti‐O bond to increase the energy band of Ti 3d states. In this way, the band gap of the doped ceramics is efficiently enhanced from 1.8 eV to 2.22 eV resulting in the large BDS. Prospectively, combined with the advantage of fine grain size, the highest recoverable energy storage density (W rec ) of 2.85 J/cm 3 is obtained at 350 kV/cm and the ultra‐high energy efficiency (η) of 95.26% is found at 200 kV/cm. Our work reveals the relationship between elements doping in B‐site and band structure, being expected to benefit for designing energy storage materials.