Lead‐Free Relaxor Ferroelectric Ceramics with Ultrahigh Energy Storage Densities via Polymorphic Polar Nanoregions Design

Abstract

One of the long-standing challenges of current lead-free energy storage ceramics for capacitors is how to improve their comprehensive energy storage properties effectively, that is, to achieve a synergistic improvement in the breakdown strength (E_b ) and the difference between maximum polarization (P_max ) and remnant polarization (P_r ), making them comparable to those of lead-based capacitor materials. Here, a polymorphic polar nanoregions (PNRs) structural design by first introducing 0.06 mol BaTiO₃ into Bi_0.5 Na_0.5 TiO₃ is proposed to construct the morphotropic phase boundary with coexisting structures of micrometer-size domains and polymorphic nanodomains, enhance the electric field-induced polarization response (increase P_max ). Then Sr(Al_0.5 Ta_0.5 )O₃ (SAT)-doped 0.94 Bi_0.5 Na_0.5 TiO₃ -0.06BaTiO₃ (BNBT) energy storage ceramics with polymorphic PNRs structures are synthesized following the guidance of phase-field simulation and rational composition design (decrease P_r ). Finally, a large recoverable energy density (W_rec ) of 8.33 J cm^-3 and a high energy efficiency (η) of 90.8% under 555 kV cm^-1 are obtained in the 0.85BNBT-0.15SAT ceramic prepared by repeated rolling process method (enhance E_b ), superior to most practical lead-free competitors increased consideration of the stability of temperature (a variation <±6.2%) and frequency (W_rec > 5.0 cm^-3 , η > 90%) at 400 kV cm^-1 . This strategy provides a new conception for the design of other-based multifunctional energy storage dielectrics.