For
(Na0.5Bi0.5)0.7Sr0.3TiO3-based (BNST) energy storage materials, a critical
bottleneck is the early polarization saturation and low breakdown
electric field (E
b), which severely limits
further development in the field of advancing pulsed power capacitors.
Herein, a strategy, via multiscale regulation, including synergistically
manipulation of the domain configuration and microstructure evolution
in BNST-based ceramics, is propounded through introducing LiTaO3(LT). The composition-driven fine domain size, as demonstrated
by macroscale (size effect and dielectric response) and mesoscale
(domains relaxor behavior) analysis, provides robust evidence of delayed
polarization saturation and large polarization difference. Theoretical
simulations and experimental results confirm that the fine grain size,
uniform grain size distribution, and insignificant secondary phase
contribute to the enhancements of E
b.
Further analyses of the intrinsic electronic structure reveal the
intrinsic mechanism for enhancing E
b via
first-principles calculations on the basis of density functional theory.
Consequently, owing to improved E
b, delayed
polarization saturation, and refined grain size, excellent comprehensive
performances [high W
rec of 5.52 J/cm3, large η of 85.68%, high hardness H of 7.06 GPa, and broad operating temperature range (20–140
°C)] are realized. We believe that these findings can provide
a thorough understanding of the origins of excellent comprehensive
performances in BNST-based ceramics as well as some guidance in the
exploration of materials with high-performance lead-free capacitors
for application in future pulsed power systems.