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Development of next-generation porous sorbents to overcome the challenges, such as low uptake capacity, slow sorption rate, and non-recyclability, associated with conventional sorbents is of utmost importance. Herein, we report the synthesis of a highly porous graphene aerogel (GA) with a unique three-dimensional hierarchical bimodal porous network of macro and meso-pores via a facile hydrothermal technique; this aerogel has sorption capacity that is more than 5 times that of conventional commercial sorbents. Fluoroalkyl silane functionalization of the GA surface results in a significant reduction in its water sorption from 20 g g−1 to 5 g g−1 due to the GA surface becoming more hydrophobic, which renders it useful in practical application to selectively remove oil from seawater. Moreover, the sorption rate of the GA for oils and organic solvents has been found to be extremely fast, and saturation of the GA is completed in a few seconds. This is attributed to its unique meso–macro bimodal porous structure with large pore channels called macro-pores or voids of various sizes ranging from 300 nm to over 10 μm, which facilitate mass transport into its inner mesopores of 14–18 nm at high rate. Finally, the GA is shown to be a highly recyclable material due to its good mechanical strength, where the oil- and organic solvent-sorbed GA can be efficiently recovered using thermal or chemical methods for several sorption–desorption cycles without significant loss in its capacity, which also makes the process cost effective and environmentally friendly.

Recyclable 3D graphene aerogel with bimodal pore structure for ultrafast and selective oil sorption from water