Phase Evolution, Filler-Matrix Interactions, and Piezoelectric Properties in Lead Zirconate Titanate (PZT)-Filled...

PZT-silsesquioxane-based 0-3 hybrid materials are prepared by mixing lead zirconate titanate (Pb(Zr,Ti)O₃; PZT) powder with a [R-SiO_3/2]_n (R = H, CH₃, CH=CH₂, C₆H₅) silsequioxane preceramic polymer. A PZT load up to 55 vol.% can be reached in the final composite. The piezoelectric and mechanical properties are investigated as a function of the filler content and are compared with theoretical models and reference samples made of the pure preceramic polymer or PZT filler. The piezoelectric response of the composites, as expressed by the relative permittivity and the piezoelectric coefficients d₃₃ and g₃₃, increases with an increasing PZT content. The bending strength of the composites ranges between 15 MPa and 31 MPa without a clear correlation to the filler content. The thermal conductivity increases significantly from 0.14 W∙m^-1∙K^-1 for the pure polymer-derived ceramic (PDC) matrix to 0.30 W∙m^-1∙K^-1 for a sample containing 55 vol.% PZT filler. From X-ray diffraction experiments (XRD), specific interactions between the filler and matrix are observed; the crystallization of the PDC matrix in the presence of the PZT filler is inhibited; conversely, the PDC matrix results in a pronounced decomposition of the filler compared to the pure PZT material.