ABSTRACT
(K,Na)NbO3 based ceramics are considered to be one of the most promising lead-free ferroelectrics replacing Pb(Zr,Ti)O3. Despite extensive studies over the last two decades, the mechanism for the enhanced piezoelectricity in multi-elements doped (K,Na)NbO3 ceramics has not been fully understood. Here, we combine temperature-dependent synchrotron x-ray diffraction and property measurements, atomic-scale scanning transmission electron microscopy, and first-principle and phase-field calculations to establish the dopant-structure-property relationship for multi-elements doped (K,Na)NbO3 ceramics. Our results indicate that the dopants induced tetragonal phase and the accompanying high-density nanoscale heterostructures with low-angle polar vectors are responsible for the high dielectric and piezoelectric properties. This work explains the mechanism of the high piezoelectricity recently achieved in (K,Na)NbO3 ceramics and provides guidance for the design of high-performance ferroelectric ceramics, which is expected to benefit numerous functional materials.
ABSTRACT
High-performance piezoelectric materials are pivotal to many electromechanical applications including piezoelectric actuators, sensors, and transducers. However, the general approach to achieve high piezoelectric properties by establishing morphotropic phase boundary (MPB) has limitation due to the weak anisotropy of the Gibbs free energy profile at the MPB region. Here, aliovalent Sm3+-doped 0.4Pb(Mg1/3Nb2/3)O3-(0.6-x)PbZrO3-xPbTiO3 piezoelectric ceramics were fabricated by a solid-state method, where the optimized piezoelectric coefficient d33 = 910 pC/N, dielectric constant εr = 4090, and Curie temperature TC = 184 °C were obtained at x = 0.352, being attributed to the synergistic contributions from the MPB and enhanced local structural heterogeneity. Rayleigh analysis was adopted to study the intrinsic and extrinsic contributions in Sm-doped PMN-PZ-PT ceramics, where the extrinsic contribution was found to be on the order of 25-67% at 4 kV/cm. Of particular significance is that a large signal d33* = 820 pm/V (at 20 kV/cm) with a minimal strain variation of 5% was achieved for a composition of x = 0.372 over the temperature range of 20-160 °C, being superior to those previously reported piezoelectric ceramic materials. This work offers a good paradigm to simultaneously achieve high piezoelectric properties with good temperature stability in ferroelectric ceramics, which have great potential for piezoelectric application at elevated temperatures.