Bi–Na–K–TiO3 and K–Na–NbO3 lead-free piezoceramics
have been widely used in next-generation
advanced pulsed-power capacitors owing to their environmental friendliness
and exceptional electromechanical and thermal behavior. However, the
enormous challenge of obtaining ultrahigh recoverable energy storage
density “W
rec” corresponding
to ultrahigh efficiency “η” has persisted and
has become a fundamental barrier inhibiting the development of lead-free
piezoceramics in cutting-edge energy storage applications. To raise
the “W
rec” and “η”
substantially, we proposed a strategy to prepare a composite of lead-free
bulk piezoceramics. To demonstrate the effectiveness of this approach,
frequency- and temperature-dependent composites of (1–x)Bi0.5Na0.25K0.25TiO3-(x)K0.5Na0.5NbO3 (BNKT-KNN) ceramics were used as a representative in this
work. (1–x)BNKT-(x)KNN piezoceramics
with sub-nanometer grains (approximately 150 nm) were prepared using
a solid-state reaction route followed by two-step sintering. The resultant
ceramics had a dense structure with minimal pores, exhibiting pseudo-cubic
symmetry and strong relaxor characteristics. The frequency- and temperature-dependent
dielectric and ferroelectric properties, along with their relaxor
behavior and energy storage properties, have been investigated. The
large “W
rec” ∼ 40
mJ/cm3 at 10 Hz and “η” ∼ 63%
at 100 Hz accomplished by applying a shallow external electric field
(35 kV/cm) for 75BNKT-25KNN ceramics is comparable to other reported
Bi–Na–K–TiO3- and K–Na–NbO3-based lead-free bulk ceramics. These outcomes demonstrate
that the (1–x)BNKT-(x)KNN
ceramics are preferred materials for advanced pulsed-power capacitors.
This study paves the way to design a novel class of piezoceramic materials
with high-energy storage applications to fulfill the stringent criteria
of modern energy storage applications.