It is challenging to achieve highly
tunable multifunctional properties
in one piezoelectric ceramic system through a simple method due to
the complicated relationship between the microscopic structure and
macroscopic property. Here, multifunctional potassium sodium niobate
[(K, Na)NbO3 (KNN)]-based lead-free piezoceramics with
tunable piezoelectric and electrostrictive properties are achieved
by controlling the long-range ferroelectric ordering (LRFO) through
antimony (Sb) doping. At a low Sb doping, the slightly distorted NbO6 octahedron and the softened B–O repulsion well maintain
the LRFO and induce plenty of nanoscale domains coexisting with a
few polar nanoregions (PNRs). Thereby, the diffused rhombohedral–orthorhombic–tetragonal
(R–O–T) multiphase coexistence with distinct dielectric
jumping is constructed near room temperature, by which the nearly
2-fold increase in the piezoelectric coefficient (d
33 ∼ 539 pC/N) and the temperature-insensitive
strain (the unipolar strain varies less than 8% at 27–120 °C)
are obtained. At a high Sb doping, the LRFO is significantly destroyed,
leading to predominant PNRs. Thus, a typical relaxor is obtained at
the ferroelectric–paraelectric phase transition near room temperature,
in which a large electrostrictive coefficient (Q
33 = 0.035 m4/C2), independent of the
electric field and temperature, is obtained and comparable to that
of lead-based materials. Therefore, our results prove that controlling
the LRFO is a feasible way to achieve high-performance multifunctional
KNN-based ceramics and is beneficial to the future composition design
for KNN-based ceramics.