A Fascinating Metallo-Supramolecular Polymer Network with Thermal/Magnetic/Light-Responsive Shape-Memory Effects Anchored by Fe3O4 Nanoparticles

Two-way shape-memory polymers (2W-SMPs) show great potential in actuating applications such as robotics due to their reversibility; indeed, multiresponsive 2W-SMPs are more expected. Inspired by the fascinating adhesion effects of mussels, we herein describe a metallo-supramolecular poly(e-caprolactone) (PCL)-based network constructed around catechol chemistry, leading to excellent thermal/magnetic/light-responsive two-way shape-memory effects (2W-SME) as well as self-healing capacity. These hybrid networks get readily self-assembled upon metal coordination interaction between superparamagnetic iron oxide nanoparticles (Fe3O4 NPs) and catechol-telechelic PCL. The incorporation of Fe3O4 NPs may act as the strong netpoints which allow the networks with excellent thermal-responsive one-way (1W) and 2W-SME, due to the ability of the semicrystalline PCL segments to present both crystallization-induced elongation (CIE) and melting-induced contraction (MIC) under constant stress. As a multifunctional medium, mor...