To meet the ever-increasing demands for pulsed power technologies, the development of lead-free dielectric ceramics with a large energy storage density (Wrec) and high energy storage efficiency (η) is crucial for enhancing the electrical performance of power capacitive devices. The conventional solid-solution, while effective in suppressing long-range order and improving energy storage performances, often results in a reduction of maximum polarization. This reduction necessitates the application of a larger electric field to obtain a relatively high Wrec. Herein, an effective strategy to enhance Wrec again via inducing Li-related defect dipoles is proposed. By introducing (Bi0.5Li0.5)TiO3 into 0.8BaTiO3-0.2BiScO3 matrix, the polarization contribution from defect dipoles together with intrinsic polarization induces an at least two-time enhancement in Pmax. Our findings indicate ∼62.9 % enhancement in the Wrec of 0.8BT-0.2BS, elevating from 2.56 J cm−3 to 4.17 J cm−3 at electrical field of 300 kV cm−1, while preserving an energy storage efficiency of 90.35 %. Furthermore, it also exhibits good thermal stability with the variations of ΔWrec < 3 % and η< 5 %. This research introduces a novel strategy for defect regulation strategy in the design of high-performance dielectric materials, which is expected to expedite the optimization of the advanced energy storage capacitors.
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