Vat photopolymerization 3D printing of transparent, mechanically robust, and self-healing polyurethane elastomers for tailored wearable sensors

As flexible sensors are soft and prone to damage in practical applications, stretchable conductors with self-healing capacity can extend their service life. However, existing vat photopolymerization (VP) 3D-printed self-healing elastomers generally have a tensile strength of less than 1 MPa, which limits the load-bearing capacity and application range of the flexible sensors. Herein, a photocurable oligomer comprising dynamic hindered urea bonds (HUBs) was synthesized to prepare self-healing elastomers. By using a surface-functionalized spherical nano-silica (Nano-SiO2) for reinforcement modification, the tensile strength and elongation at break of the 3D-printed elastomer were enhanced by 73.7% and 111.3%, respectively, without compromising the transparency and photopolymerization rate. The fractured elastomer exhibited a high tensile strength of 5.44 MPa and a stretchability of 372% after self-healing. Subsequently, a stretchable ionic conductive elastomer (SICE) with high transparency and self-healing properties was developed by incorporating ionic liquids into the 3D-printed elastomer. The high resolution of VP-based 3D printing allowed the construction of pyramid-Kelvin lattice microstructures in the pressure sensor, which enhanced the pressure sensitivity of the sensor several times compared to the pyramid structure. In addition, combining Voronoi tessellation and kirigami art to fabricate tailored wearable sensors with smart structures, broadens the application range and improves the wearing comfort of the sensors.