Stimulus-Responsive Graphene with Periodical Wrinkles on Grooved Microfiber Arrays: Simulation, Programmable Shape-Shifting, and Catalytic Applications

This work demonstrates a facile fabrication of stimulus-responsive, periodically wrinkled graphene sheets on grooved microfiber arrays with fast and reversible shape change, multiresponsiveness, and programmable deformation, with the aid of finite element analysis (FEA). The cellulose acetate (CA) microfibers, endowing responsiveness to humidity and solvents, are designed to grooved shape and assembled into a well-aligned fibrous mat by electrospinning. Under the guidance of FEA simulation, the stiff reduced graphene oxide (RGO) sheets, serving as a photoresponsive component, could ably bind on grooved CA microfibers with favorable interlocked interfacial-structure. Through simple direct-writing and hot-pressing, the grooved CA arrays interlocked the conformal RGO sheets by water-induced self-clamping, and enabled the generation of periodic wrinkles within RGO sheets to maximize interfacial areas. By simply adjusting the orientation of written RGO patterns relative to uniaxial CA microfibers, programmed and omnidirectional shape-shifting were obtained to minimize strain energy, consisting with the dynamic deformation process simulated by FEA. Upon remote light or contactless humidity stimuli, the RGO/CA mat shows a rapid response (≤1 s), large amplitude (angle change ≥150°, 1.62 cm–1), sophisticated 3D motions, and lifts objects that weigh 12.7-times its own weight up to over 1/3 of own height within 1 s. After loading catalytical nanoparticles, the RGO/CA mat could rapidly move to the targeted position by continuous crawling even on a slippery surface, and served as a microchannel reactor to trigger a reaction in built-in microchannels with suppressing catalyst leaching while accelerating reaction kinetics by both nanoconfinement and photothermal effect.