Optimized Polyurethane/CNTs Composite for Stress-Free Two-Way Shape Memory via Training Enhancement

Thermally responsive shape memory polymer materials are the most widely used type of intelligent materials and have found applications in numerous fields. However, their practical utility is often limited by poor heat conduction. Carbon nanotubes (CNTs), renowned for their exceptional thermo-conductive and photothermal properties, provide a promising solution. In this study, CNTs were integrated into polyurethane prepared by stepwise polymerization method, using hydroxyl terminated polycaprolactone (PCL-diOH), poly(ethylene glycol) (PEG) and hexamethylene diisocyanate (HDI). The resulting polyurethane composite material exhibits remarkable mechanical strength, enhanced thermal conductivity, and superior shape memory performance. Notably, it demonstrates a form of training enhancement phenomenon, which shows higher mechanical properties. And the composite could achieve stress-free two-way shape memory behavior after cyclic stretching process. Additionally, this composite material can exhibit “vitrimer” material properties at higher temperatures (110 °C), allowing for shape reprogramming. The carbon nanotube-reinforced composite material can achieve remote and precise manipulation under light stimulation. By combining the composite material with a metal thermally conductive layer, a multi-layer structure with shape memory properties can be prepared, which can achieve two-way shape memory behavior under electrical and light stimulation, further expanding the application potential of the composite material in the real world.