Superior Energy-Storage Performances under a Moderate Electric Field Achieved in Antiferroelectric-like NaBiTiO-Based Relaxor Ferroelectric Ceramics by a Synergistic Optimization Strategy.

The progress of power systems and electronic devices promotes the development of lead-free dielectric energy-storage material. Particularly, NaBiTiO-based ferroelectric ceramics featuring large spontaneous polarization as well as wide dielectric adjustability and stability are highly recognized as promising candidates. However, their large remanent polarization () and low electric breakdown strength () result in unsatisfactory recoverable energy density () and/or energy conversion efficiency (η), severely restricting their energy-storage applications. Herein, an effective synergistic optimization strategy has been proposed to gain superior energy-storage performances. Interestingly, the antiferroelectric-like (AFE-like) (1 - )(NaBiSrTiO)-Bi(MgZr)O ( = 0.00, 0.05, 0.10, 0.15, and 0.20) relaxor ferroelectric (RFE) ceramics were constructed via the phase structure, the polar structure, and the defect dipole modulations. With Bi(MgZr)O increasing, the slim and pinched polarization-electric field hysteresis () loops become remarkably similar to the double-like loops characterized by AFEs. Meanwhile, the strengthened and delayed polarization saturation were also realized due to the enlarged band gap, refined grain size, and reduced free energy barrier. Consequently, superior energy-storage performances were achieved in this work. Noticeably, a large of 5.00 J/cm and a high η of 90.09% were realized in 0.85(NaBiSrTiO)-0.15Bi(MgZr)O RFE ceramics at a moderate electric field of 340 kV/cm. Additionally, excellent energy-storage and/or charge-discharge reliabilities in frequency (1-500 Hz), temperature (20-140 °C), and fatigue cycle (1-50,000) were confirmed. These satisfactory results not only indicate the promising prospects of 0.85(NaBiSrTiO)-0.15Bi(MgZr)O RFE ceramics in the dielectric energy-storage field but also verify the effectiveness of the synergistic optimization strategy proposed in this work.