Hierarchical aerogels based on cellulose nanofibers and long-chain polymers for enhancing oil–water separation efficiency

The hydrophobic chain length of biomass-based aerogels used for oil–water separation was evaluated as a major parameter influencing the aerogels' hydrophobicity. The properties of the porous structure were enhanced by the hierarchical assembly of the aerogels with biopolymeric structural units and polymer mineralization. The cellulose network was strengthened through silanization, and the nanocellulose network was further enhanced through coating with mineralizers containing long-chain hydrophobic molecules. Interfacial engineering was employed to establish multiscale interactions through the freeze-drying-induced modification of cellulose nanofibers and mineralized coatings of long-chain alkyl polymers. The resulting hierarchically structured aerogel exhibits low density (11.4 kg/m3), excellent mechanical compression properties across a wide temperature range (capable of enduring 100 cycles of compression), high porosity (99.2%), superhydrophobicity (152°), and recyclability. It maintains a 57.9% adsorption rate even after 40 adsorption–desorption tests, while also preserving its shape integrity. Moreover, it can be recycled and reused. At a temperature of 700 °C, the mass loss was only 44.47%, with excellent thermal stability. The aerogel can reduce oil pollutants in the ocean by adsorption, recover oil resources, and protect the natural environment. The assembly and optimization of nanofibrous matrix interfaces through the mineralization of long-chain polymers enhanced the performance of functionalized cellulose-based aerogels.