Piezoelectric energy harvesters (PEHs) with porous structures, such as piezoelectric elastic sponges, exhibit high force-to-electricity conversion efficiencies owing to their excellent compression recovery properties. However, conventional preparation methods are limited to producing bulk-form sponge-like PEHs and fail to create more elaborate three-dimensional (3D) structures that could enhance conversion efficiency. Herein, we invent a composite ink consisting of waterborne polyurethane (WPU), barium titanate (BTO), and cellulose nanofibers (CNFs) that is suitable for direct ink writing (DIW) 3D printing. This ink, when coupled with freeze-drying, allows the customization of piezoelectric sponges with functional 3D structures. The printed lattice sponge exhibits remarkable compression recovery of 70% and a notably high relative sensitivity of 9.83 mV/kPa*wt % (where *wt % denotes the BTO content) across a wide pressure range of 2.98-37 kPa, which is approximately three times broader than those of other composite piezoelectric pressure sensors based on BTO or piezoceramic (PZT) materials. Furthermore, a customized 3D piezoelectric sponge with a "boomerang" configuration is utilized as an anisotropic bending sensor on the wrist for intelligently monitoring the stroke posture and programming scientific training for table tennis players. This study highlights a versatile strategy for constructing elastic sponges with high piezoelectricity and designing 3D PEH functional structures that can be applied to flexible self-powered intelligent sensing systems.
Keywords: 3D printing; barium titanate; composite sponge; flexible sensor; piezoelectricity.