Comparison of different sintering aids in cold sinter-assisted densification of lead zirconate titanate

Ceramics such as lead zirconate titanate (PZT) tend to dissolve incongruently, and thus pose a challenge in the cold sintering process. Moist lead nitrate has previously been shown to enable a cold sinter-assisted densification of PZT by a viscous phase sintering mechanism. In this paper, lead acetate trihydrate is demonstrated to lower the required temperature of the cold sintering step to 200°C. This densification process was described as a two-step process: cold sintering of PZT with lead acetate trihydrate and post-annealing the as-cold sintered PZT ceramics. Unlike in the case of lead nitrate, PZT densification with lead acetate trihydrate occurs by a liquid phase assisted sintering mechanism, leading to an as-cold sintered relative density of 84% at 200°C. After performing a post-anneal step at 900°C, >97% relative densities were achieved in samples that were cold sintered with lead acetate trihydrate. This step not only densified PZT but also refined the grain boundaries. In the post-annealed samples, the room-temperature relative permittivity at 100 Hz was ~1600, slightly higher than that reported in samples that used lead nitrate as a sintering aid; the loss tangent was about 3.8%. For measurements at 10 Hz, the remanent polarization in both cases was ~28 µC/cm². Both Rayleigh analysis and aging studies showed that a higher irreversible contribution to the permittivity exists in samples that used lead nitrate as a cold sintering aid.