Millisecond Response of Shape Memory Polymer Nanocomposite Aerogel Powered by Stretchable Graphene Framework

Shape memory polymers (SMPs) change shapes as-designed through altering the chain segment movement by external stimuli, promising wide uses in actuators, sensors, drug delivery, and deployable devices. However, the recovery speed of SMPs is still far slower than the benchmark shape memory alloys (SMAs), originating from their intrinsic poor heat transport and retarded viscoelasticity of polymer chains. In this work, monolithic nanocomposite aerogels composed of bicontinuous graphene and SMP networks are designed to promote the recovery time of SMP composites to a record value of 50 ms, comparable to the SMA case. The integration of a stretchable graphene framework as a fast energy transformation grid with ultrathin polycaprolactone nanofilms (tunable at 2.5-60 nm) enables the rapid phase transition of SMPs under electrical stimulation. The graphene-SMP nanocomposite aerogels, with a density of ∼10 mg cm-3, exhibit a fast response (175 ± 40 mm s-1), large deformation (∼100%), and a wide response bandwidth (0.1-20 Hz). The ultrafast response of SMP nanocomposite aerogels confers extensive uses in sensitive fuses, micro-oscillators, artificial muscles, actuators, and soft robotics. The design of bicontinuous ultralight aerogels can be extended to fabricate multifunctional and multiresponsive hybrid materials and devices.