Boosting Capacitive Performance of Lead-Free Relaxor Ferroelectrics by Introducing a Linear Dielectric

As an important core component used in high-power pulse electronic systems, dielectric ceramic capacitors have gained great interest because of their ultrahigh powder density (PD) and fast discharge speed (t0.9). However, inferior energy storage performance (ESP) greatly limits the development of energy storage devices with the requirement of miniaturization and integration. Herein, we propose a feasible approach to introduce linear dielectric CaTiO3 (CT) into (Bi0.5Na0.5)TiO3 (BNT) for the design of engineered relaxor ferroelectrics to tune ESP at the grain, domain, and macroscopic scales. The results demonstrate that introducing CT generates enhanced relaxor behavior with highly dynamic polar nanoregions, refines grain size, and suppresses dielectric loss, synergistically yielding increased breakdown strength, negligible remnant polarization, and a nearly linear po-larization hysteresis loop. Consequently, superior ESP is achieved in BNT-0.3CT relaxor ferroelectric ceramics with a large energy density (-5.65 J/cm3) and a high efficiency (-88.1 %). Based on CT-induced merits, the excellent temperature/frequency/cycling stabilities and remarkable charge-discharge properties featuring a high PD of 200.4 MW/cm3, high discharge energy density of 2.27 J/cm3 and ultrashort t0.9 of 58 ns of the designed ceramics broaden the actual application prospects. This work demonstrates that introducing linear dielectric CT holds great promise for developing high-performance energy storage dielectrics.