Lead‐free Na 0.5 K 0.5 NbO 3 (NKN) piezoelectric ceramics were fairly well densified at a relatively low temperature under atmospheric conditions. A relative density of 96%–99% can be achieved by either using high‐energy attrition milling or adding 1 mol% oxide additives. It is suggested that ultra‐fine starting powders by active milling or oxygen vacancies and even liquid phases from B‐site oxide additives mainly lead to improved sintering. Not only were dielectric properties influenced by oxide additives, such as the Curie temperature ( T c ) and dielectric loss ( D ), but also the ferroelectricity was modified. A relatively large remanent polarization was produced, ranging from 16 μC/cm 2 for pure NKN to 23 μC/cm 2 for ZnO‐added NKN samples. The following dielectric and piezoelectric properties were obtained: relative permittivity ɛ T 33 /ɛ 0 =570–650, planar mode electromechanical coupling factor, k p =32%–44%, and piezoelectric strain constant, d 33 =92–117 pC/N.
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