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Antiferroelectrics (AFEs) are promising candidates in energy-storage capacitors, electrocaloric solid-cooling, and displacement transducers. As an actively studied lead-free antiferroelectric (AFE) material, NaNbO3 has long suffered from its ferroelectric (FE)-like polarization-electric field (P-E) hysteresis loops with high remnant polarization and large hysteresis. Guided by theoretical calculations, a new strategy of reducing the oxygen octahedral tilting angle is proposed to stabilize the AFE P phase (Space group Pbma) of NaNbO3. To validate this, we judiciously introduced CaHfO3 with a low Goldschmidt tolerance factor and AgNbO3 with a low electronegativity difference into NaNbO3, the decreased cation displacements and [BO6] octahedral tilting angles were confirmed by Synchrotron X-ray powder diffraction and aberration-corrected scanning transmission electron microscopy. Of particular importance is that the 0.75NaNbO3−0.20AgNbO3−0.05CaHfO3 ceramic exhibits highly reversible phase transition between the AFE and FE states, showing well-defined double P-E loops and sprout-shaped strain-electric field curves with reduced hysteresis, low remnant polarization, high AFE-FE phase transition field, and zero negative strain. Our work provides a new strategy for designing NaNbO3-based AFE material with well-defined double P-E loops, which can also be extended to discover a variety of new lead-free AFEs.

As an efficient and economical way of dealing with organic pollutants, piezo-photocatalysis has attracted great interest. In this work, we demonstrated that ferroelectricity and Schottky heterojunction engineering could significantly enhance the piezo-photocatalytic activity of AgNbO3. The poled 20 mol % K+ doped AgNbO3 disclosed its superior piezo-photocatalytic activity of 0.131 min–1 for 10 mg·L–1 RhB, which is 7.8 times of the pristine one under the condition of illumination only. The designed piezo-photocatalyst also exhibited good piezo-photocatalytic stability after four cycles. These merits are attributed to the built-in electric field associated with the large spontaneous polarization and low coercive field originated from the stable ferroelectric state after ferroelectricity engineering, plus with the electron trapper effect of the in situ precipitated metal Ag particles. Our work not only provides a promising piezo-photocatalyst for degrading organic contaminants but also paves a good way for developing high piezo-photocatalytic activity catalysts.