Fabricating Remote-Controllable Dynamic Ionomer/CNT Networks via Cation–π Interaction for Multi-Responsive Shape Memory and Self-Healing Capacities

Shape memory polymers (SMPs) with remotely controllable triggering capabilities are crucial for actuating applications in biomedical and aeronautic devices. This work presents a novel ionomer/carbon nanotube (CNT) composite network with exceptional remotely controllable shape memory effects (SMEs) and self-healing capabilities. By integrating quaternary ammonium (QA) units covalently bonded to crystalline polycaprolactone (PCL) segments through a chain extension reaction, we not only enabled the formation of ion clusters that act as netpoints in PCLQA ionomers to achieve superior SMEs, but also facilitated the generation of cation-π interactions when the multiresponsive CNTs were incorporated into the PCLQA ionomer matrix. This resulted in a robust physical PCLQA@CNT network stabilized by ionic clusters and cation-π interactions, along with significantly enhanced CNT dispersion. The PCLQA@CNT composites demonstrated remarkably improved mechanical performance (tensile strength, σ_b > 40 MPa; elongation at break, ε_b > 1900%), excellent thermally induced SME (shape fixity ratio of 99.6% and shape recovery ratio of 92.3%), and exceptional antibacterial effects (>99% against <i>Escherichia coli</i> and <i>Staphylococcus aureus</i>). Furthermore, the physical dynamic interactions endowed PCLQA@CNT networks with reproducibility and welding capability. The remotely controllable shape memory and self-healing behaviors via NIR and electrical stimulation were verified and demonstrated. This work paves the way for developing remotely controllable shape memory materials for advanced intelligent devices and applications.