High Aspect Ratio Carboxylated Cellulose Nanofibers Cross-linked to Robust Aerogels for Superabsorption–Flocculants: Paving Way from Nanoscale to Macroscale

Charged nanocellulose (NC) with a high aspect ratio (larger than 100) extracted from animal or bacterial cellulose and chemical cross-linked NC aerogels have great promising applicability in material science, but facile fabrication of such NC aerogels from plant cellulose by physical cross-linking still remains a major challenge. In this work, carboxylated cellulose nanofiber (CNF) with the highest aspect ratio of 144 was extracted from wasted ginger fibers by a simple one-step acid hydrolysis. Our approach could easily make the carboxylated CNF assemble into robust bulk aerogels with tunable densities and desirable shapes on a large scale (3D macropores to mesopores) by hydrogen bonds. Excitingly, these CNF aerogels had better compression mechanical properties (99.5 kPa at 80% strain) and high shape recovery. Moreover, the CNF aerogels had strong coagulation–flocculation ability (87.1%), removal efficiency of MB dye uptake (127.73 mg/g), and moderate Cu2+ absorption capacity (45.053 mg/g), which were due to assistance mechanisms of charge neutralization, network capture effect, and chain bridging of high aspect ratio carboxylated CNF. This provided a novel physical cross-linking method to design robust aerogels with modulated networked structures to be a general substrate material for industrial applications such as superabsorbent, flocculation, oil–water separation, and potential electrical energy storage materials.