Magnetic- and light-responsive shape memory polymer nanocomposites from bio-based benzoxazine resin and iron oxide nanoparticles

Shape memory polymers (SMPs) are a class of smart materials that can be programmed to recover from temporary shape to permanent shape by applying external stimuli (temperature, magnetic field, light, electric field, and moisture, etc.). This unique property of SMPs makes them an appealing candidate in application for soft robotics, such as smart actuators, artificial muscles, and biomedical devices. In this contribution, we have developed multi-stimuli-responsive SMPs from bio-based benzoxazine resin and iron oxide nanoparticles (Fe₃O₄ NPs) that could be actuated by magnetic field and light. The nanocomposites were characterized by infrared spectroscopy, in which molecular interaction between benzoxazine/epoxy copolymers and Fe₃O₄ NPs was observed. Effects of nanoparticle content (0–5 wt%) on magnetic, mechanical, thermal, and thermo-mechanical properties of nanocomposites were investigated. Shape memory performance of nanocomposites was significantly improved with incorporation of Fe₃O₄ NPs. Shape fixity increased from 85% of neat copolymers to 93% of copolymers filled with 3 wt% Fe₃O₄ NPs, while shape recovery increased from 94% to 98%. Moreover, shape fixity could be done without external force contact by 808 nm-light actuation and magnetic attraction, due to photothermal and magnetic properties of nanocomposites. Shape recovery was tested under actuation by magnetic field. The highest shape recovery ratio was 99% within 26 s for copolymers filled with 5 wt% Fe₃O₄ NPs. Lastly, preliminary application of nanocomposites was demonstrated as they could push a 1 g-object within 10 s of actuation by magnetic field. In overall, these nanocomposites with multi-stimuli-responsive shape memory property had a good potential to be applied for soft robotics.