This work presents a new process to print piezoelectric polymer-based sensors through additive manufacturing via three-dimensional (3D) printing technology. 3D printing has become an efficient method to fabricate devices with complex geometric structures and embedded functionalities. The motivation of this research was to explore a path towards fully 3D printed multifunctional thin and flexible sensing devices. The 3D printed methods used were Fused Deposition Modelling and Direct Ink Writing. A fully 3D printed sensor consisting of a (2.54 cm × 2.54 cm) poly(vinylidene fluoride) (PVdF) film with thickness in the range of ∼250 μm to 350 μm was sandwiched between two fast-drying silver paint printed electrodes with thickness ranging from ∼10 μm to 50 μm. The arithmetic average roughness, Ra, of typical printed PVdF profiles with and without printed silver electrodes was ∼12.9 μm and ∼7.3 μm, respectively. Silver electrodes were printed to facilitate contact poling and to collect charges generated due to piezoelectricity. The average piezoelectric activity of printed unpoled films was 7.13 pC/N. The polarization in the printed PVdF films was realized by conventional contact poling at elevated temperatures (100, 110, 120 and 130 °C, respectively) with step increased electric fields, which were varied from 0.4 MV/m to 14 MV/m at 1 MV/m increments. To perform contact poling, PVdF films were immersed in mineral oil and a controlled voltage was applied to electrodes on one side while electrodes on the opposite side were grounded. The extrusion process during 3D printing and the subsequent contact poling process enabled the phase transition from the thermally stable α-phase to the piezoelectric active β-phase and the rearranging of the dipole alignments. The efficiency of poling was evaluated through measurement of the average value of the charge generated by six poled PVdF films in response to mechanical input increasing from 0.29 N to 1.91 N with ∼0.27 N increments. The highest average piezoelectric activity obtained was 59.2 pC/N, and a single device of 96.44 pC/N, at step increased poling voltages up to 3.5 kV under a fixed temperature 120 °C. The results demonstrate that by increasing the poling voltages and time, a higher piezoelectric activity (about 8 times compared to unpoled films) was achieved, indicating improvement of the β-phase content. This study provides a new method for continuous and direct printing of piezoelectric devices from PVdF polymeric filament. This technology opens a new path towards fully 3D printed free-form structured functional materials for sensing applications.

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