Large piezoelectricity in NaNbO3-based lead-free ceramics via tuning oxygen octahedral tilt

The development of high-performance lead-free piezoceramics for replacing Pb-based perovskites has attracted lots of attention, and comparable room-temperature piezoresponse has been realized in (Na,K)NbO3 and BaTiO3-based ceramics with local structure heterogeneity via adjusting polymorphic phase boundary. In this work, a new method of oxygen octahedron tilt design is used in NaNbO3-based lead-free ceramics, which usually shows complex oxygen octahedron tilt information inherited from NaNbO3. The substitution of Ba(Fe0.5Nb0.5)O3 and BaTiO3 with high tolerance factor into NaNbO3 leads to a gradual elimination of anti-parallel cation displacement and anti-phase tilt along the three axes; as a result, a single tetragonal phase with P4bm space group and only in-phase tilt along c axis is achieved in 0.88NaNbO3–0.04Ba(Fe0.5Nb0.5)O3–0.08BaTiO3 ceramic. Accompanying the decreased oxygen octahedral tilt degree, a drastically improved d33 up to 367 pC N−1 (over ten times that of NaNbO3 ceramic) is obtained, reaching a record high in NaNbO3-based lead-free ceramics. Together with temperature insensitive piezoresponse originating from thermally stable oxygen octahedral tilt structure, the studied NaNbO3-based materials show large potential for replacing Pb-based ceramics in some electronic devices. The oxygen octahedron tilt engineering would be used for designing more high-performance lead-free ceramics with high piezoresponse and excellent thermal stability simultaneously.