Microstructure and Electrical Properties of Pb[(Mg,Mn)Nb]O3-Pb(Zr,Ti)O3 Piezoelectric Ceramics

Phase evolution, microstructure and the electrical properties such as $k_p$ and $Q_m$ of $Pb(Mg_{1/3}Nb_{2/3})O_3[PMN]-Pb(Mn_{1/3}Nb_{2/3})O3[PM quaternary system were investigated within the compositional ranges $0{\leq}y{\leq}0.125$, y+z=0.125, and $0.39{\leq}x{\leq}0.54$ of the formula $Pb_{0.97}Sr_{0.03}[Mg_{1/3}Nb_{2/3})_y\;(Mn_{1/3}Nb_{2/3})_z\;(Zr_{x}Ti_{1-x})_{1-(y+z)}]O_3$. In the case of increasing Mn/(Mg+Mn) ratio for a fixed Zr/Ti ratio of 47.5/52.5, phase relation remained unchanged but the grain size drastically decreased, and the electrical properties changed as following: both $k_P$ and $Q_m$ reached the peak values at $Mn/(Mg+Mn)\cong0.3l7$ and gradually decreased; $\varepsilon33^T$ showed a monotonic decrease; P-E hysteresis loop gradually changed to asymmetrical one, and $E_i$ increased in correspondence. With increasing Zr/Ti ratio for a fixed Mn/(Mg+Mn) ratio of 0.317, on the contrary, the cell parameter $(\alpha^2c)^{1/3}$ gradually increased, and tetragonal-rhombohedral morphotropic phase boundary appeared in the range of $51/49{\leq}Zr/Ti{\leq}54/46$. the meantime, the grain size substantially increased, and the electrical properties changed as following: $k_P$ and $\varepsilon33^T$ reached peak values at Zr/Ti=51/49 and 48/52, respectively, and then gradually decreased; change of $Q_m$ was adverse to $k_P$; both $E_C\;and\;E_i$ considerably decreased while $P_S$ moderately increased. For the system 0.125(PMN+PM'N)-0.875PZT studied, the composition Mn/(Mg+Mn)=0.3l7 and Zr/Ti=51/49 revealed some promising electrical properties for piezoelectric transformer application such as $k_P=0.58,\;Q_m\cong1000$, and $\varepsilon^T_{33}=970$, as well as dense and fine-grained microstructure.