Synergistic Optimization of Energy Storage Density of PYN-Based Antiferroelectric Ceramics by Composition Design and Microstructure Engineering

PbYb_0.5 Nb_0.5 O₃ (PYN)-based ceramics, featured by their ultra-high phase-switching field and low sintering temperature (950 °C), are of great potential in exploiting dielectric ceramics with high energy storage density and low preparation cost. However, due to insufficient breakdown strength (BDS), their complete polarization-electric field (P-E) loops are difficult to be obtained. Here, to fully reveal their potential in energy storage, synergistic optimization strategy of composition design with Ba²⁺ substitution and microstructure engineering via hot-pressing (HP) are adopted in this work. With 2 mol% Ba²⁺ doping, a recoverable energy storage density (W_rec ) of 10.10 J cm^-3 and a discharge energy density (W_dis ) of 8.51 J cm^-3 can be obtained, supporting the superior current density (C_D ) of 1391.97 A cm^-2 and the outstanding power density (P_D ) of 417.59 MW cm^-2 . In situ characterization methods are utilized here to reveal the unique movement of the B-site ions of PYN-based ceramics under electric field, which is the key factor of the ultra-high phase-switching field. It is also confirmed that microstructure engineering can refine the grain of ceramics and improve BDS. This work strongly demonstrates the potential of PYN-based ceramics in energy storage field and plays a guiding role in the follow-up research.