Bioinspired Assembly of Carbon Nanotube into Graphene Aerogel with “Cabbagelike” Hierarchical Porous Structure for Highly Efficient Organic Pollutants Cleanup

Nowadays, physical absorption has become a feasible method offering an efficient and green route to remove organic pollutants from the industrial wastewater. Inspired by polydopamine (PDA) chemistry, one-dimensional PDA-functionalized multiwalled carbon nanotubes (MWCNT-PDA) were creatively introduced into graphene aerogel framework to synthesize a robust graphene/MWCNT-PDA composite aerogel (GCPCA). The whole forming process needed no additional reducing agents, significantly reducing the contamination emissions to the environment. The GCPCA exhibited outstanding repeatable compressibility, ultralight weight, as well as hydrophobic nature, which were crucial for highly efficient organic pollution absorption. The MWCNTs in moderate amounts can provide the composite aerogels with desirable structure stability and extra specific surface area. Meanwhile, the eventual absorption performance of GCPCAs can be improved by optimizing the microporous structure. In particular, a novel "cabbagelike" hierarchical porous structure was obtained as the prefreezing temperature was decreased to -80 °C. The miniaturization of pore size around the periphery of GCPCA enhanced the capillary flow in aerogel channels, and the super-absorption capacity for organic solvents was up to 501 times (chloroform) its own mass. Besides, the GCPCAs exhibited excellent reusable performance in absorption-squeezing, absorption-combustion, and absorption-distillation cycles according to the characteristic of different organic solvents. Because of the viable synthesis method, the resulting GCPCAs with unique performance possess broad and important application prospects, such as oil pollution cleanup and treatment of chemical industrial wastewater.