BaHf_0.05Ti_0.95O₃ Ceramics from Sol-Gel and Solid-State Processes: Application to the Modelling of Piezoelectric...

A typical piezoelectric energy harvester is a bimorph cantilever with two layers of piezoelectric material on both sides of a flexible substrate. Piezoelectric layers of lead-based materials, typically lead zirconate titanate, have been mainly used due to their outstanding piezoelectric properties. However, due to lead toxicity and environmental problems, there is a need to replace them with environmentally benign materials. Here, our main efforts were focused on the preparation of hafnium-doped barium titanate (BaHf_xTi_1-xO₃; BHT) sol-gel materials. The original process developed makes it possible to obtain a highly concentrated sol without strong organic complexing agents. Sol aging and concentration can be controlled to obtain a time-stable sol for a few months at room temperature, with desired viscosity and colloidal sizes. Densified bulk materials obtained from this optimized sol are compared with a solid-state synthesis, and both show good electromechanical properties: their thickness coupling factor k values are around 53% and 47%, respectively, and their converse piezoelectric coefficient d33∗ values are around 420 and 330 pm/V, respectively. According to the electromechanical properties, the theoretical behavior in a bimorph configuration can be simulated to predict the resonance and anti-resonance frequencies and the corresponding output power values to help to design the final device. In the present case, the bimorph configuration based on BHT sol-gel material is designed to harvest ambient vibrations at low frequency (<200 Hz). It gives a maximum normalized volumetric power density of 0.03 µW/mm³/Hz/g² at 154 Hz under an acceleration of 0.05 m/s².