New Aurivillius ferroelectrics Na0.5La0.5Bi2Nb2−xWxO9 (NLBN-W, x = 0, 0.01, 0.02, 0.03, and 0.05) by lanthanum (La3+) and tungsten (W6+) co-substitution were prepared by using a solid-state reaction process. The crystal structure of Na0.5La0.5Bi2Nb1.98W0.02O9 (NLBN-W-0.02) was refined by the Rietveld method with powder X-ray diffraction at room temperature and it was confirmed to be a two-layer Aurivillius oxide with an orthorhombic space group A21am (a = 5.48754(8) Å, b = 5.47967(9) Å and c = 24.8523(4) Å). The ferroelectric to paraelectric phase transition temperature (Tc) of NLBN-W-0.02 is around 501 °C, with prominent relaxation behavior. The NLBN-W-0.02 ceramics have a high piezoelectric coefficient (d33 = 31 pC N−1) and large remnant polarization (Pr = 15.1 μC cm−2). The decrease in Pr for the NLBN-W-0.02 ceramics after 107 switching cycles at 40 and 120 °C is only 2 and 9%, respectively.
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