A facile and scalable approach to prepare multilayered graphene coated carbon nanofiber (G-CNF) foam has been demonstrated for oil/chemical solvent spill clean-up applications. 2D electrospun polyacrylonitrile/itaconic acid (PANIA) membrane was converted into a nature inspired three-dimensional (3D) aerogel networks self-assembled by a gas foaming method. The 3D nanofiber foams were then coated with Graphene Oxide (GO) and carbonised into G-CNF foam. These foams display highly interconnected network; mimicking the features of chicken feather and demonstrated the synergistic properties of graphene and carbon nanofibers. These 3D foams were light weight, resilient and exhibited fire-resistance properties. The design features of the G-CNF foams comprise of interconnected carbon nanofiber layers leading to high specific surface area that contributed towards oil and solvents sorption properties. The G-CNF foams perform high saturation sorption capacity (86–153 g g−1) toward a range of oils and organic solvents and demonstrated sustained sorption capabilities even after 11 cycles. In addition, the topology of the G-CNF surface and the morphology of the nanofiber foam were simulated and further studied using microstructure computational modelling and numerical analysis, which altogether showed that a significant enhancement in the surface area-to-volume ratio resulting from the coated graphene on the G-CNF foam.
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