A Breathable, Highly Sensitive, and Wearable Piezoresistive Sensor with a Wide Detection Range Based on Gradient Porous PU@MXene/CNT Film for Electronic Skin

Developing flexible sensors that combine high sensitivity, a wide detection range, and comfortable wearability remains a key challenge in the development of electronic skin. This study presents a breathable, highly sensitive, and wearable piezoresistive sensor based on the preparation of hierarchical microporous PU@MXene + CNT films and single-sided electrodes using a simple and effective method. Distilled water was used as a non-solvent to induce the separation of polyurethane films (PU) with different mass fractions, forming a gradient porous structure with inconsistent pore morphologies in the upper and lower layers. Three-dimensional structure analysis of the hierarchical porous films with varying gradients, conducted using computed tomography, revealed that the porous structures formed after phase separation of PU solutions with different mass fractions exhibited different morphologies. As the mass fraction increased, the pore size, pore volume, and porosity gradually decreased while the surface area gradually increased. The greater the gradient of the constructed porous film, the more significant the difference between the upper- and lower-layer structures. A flexible sensor prepared using the PU@MXene + CNT porous film with the largest gradient exhibited excellent sensitivity in a wide detection range from 0.7 to 20 kPa, which was higher than that of porous films with other gradients, demonstrating high stability (>8000 cycles). The air permeability and moisture permeability of PU@MXene + CNT with the largest gradient were 0.9922 L/m²/s and 1123.6 g/m²/day, respectively, and these values were 1.35 and 4.40 times those of the non-porous film. Therefore, the constructed flexible piezoresistive sensor with a gradient porous structure had both high sensitivity and wide detection range, as well as good air and moisture permeability. Finally, the sensor successfully monitored human movements, including throat activity, finger motions, and arm bending, demonstrating its potential for wearable electronic applications.