Healable Strain Sensor Based on Tough and Eco-Friendly Biomimetic Supramolecular Waterborne Polyurethane

Stretchable sensors are essential for flexible electronics, which can be made with polymer elastomers as the matrix. The main challenge in producing practical devices is to obtain polymers with mechanical stability, eco-friendliness, and self-healing properties. Herein, we introduce urea bonds and 2-ureido-4[1H]-pyrimidinone (UPy) to synthesize tailored waterborne polyurethanes (WPU-UPy-x) with a hierarchical hydrogen bond (H-bond). Accordingly, sound tensile performance (strength: 53.33 MPa, toughness: 128.97 MJ m^-3), satisfying deformation recovery, and good self-healing capability of the WPU-UPy-x film are demonstrated. With atomic force microscope characterization, we find that UPy groups contribute to the highly improved microphase separation of WPU-UPy-x, responsible for good mechanical properties. As a proof of concept, a strain sensor is successfully configured, thanks to the good interfacial interactions between the polyurethane matrix and the Ti₃C₂T_x MXene conductive filler, which features sensitive and stable performance for monitoring diverse human and mechanical motions. Intriguingly, this sensor is capable of self-healing after cutting and displays well-retained sensitivity to detect the stretched signal. The as-proposed design concept for healable and sensitive strain sensors can shed light on future wearable electronics.