Cold sintering and electrical characterization of lead zirconate titanate piezoelectric ceramics

This paper describes a cold sintering process for Pb(Zr,Ti)O3 ceramics and the associated processing-property relations. Pb(Zr,Ti)O3 has a very small, incongruent solubility that is a challenge during cold sintering. To circumvent this, a Pb(NO3)2 solution was used as the transient liquid phase. A bimodal lead zirconate titanate powder was densified to a relative density of 89% by cold sintering at 300 °C and 500 MPa. After the cold sintering step, the permittivity was 200, and the dielectric loss was 2.0%. A second heat-treatment involving a 3 h anneal at 900 °C increased the relative density to 99%; the resulting relative dielectric permittivity was 1300 at room temperature and 100 kHz. The samples showed well-defined ferroelectric hysteresis loops, having a remanent polarization of 28 μC/cm2. On poling, the piezoelectric coefficient d33 was ∼200 pC/N. With a 700 °C 3 h post-annealing, samples show a lower room temperature relative permittivity (950 at 100 kHz), but a 24 h hold time at 700 °C produces ceramics where there is an improved relative dielectric constant (1050 at 100 kHz).