Anisotropic cellulose nanocrystalline sponge sheets with ultrahigh water fluxes and oil/water selectivity.

Oily sewage caused by oil spill accidents has become a severe problem in the last decades. Hence, two-dimensional sheet-like filter materials for oil/water separation have received widespread attention. Porous sponge materials were developed using cellulose nanocrystals (CNCs) as raw materials. They are environmentally friendly and easy to prepare, with high flux and separation efficiency. The 1,2,3,4-butane tetracarboxylic acid cross-linked anisotropic cellulose nanocrystalline sponge sheet (B-CNC) exhibited ultrahigh water fluxes driven by gravity alone, depending on the aligned structure of channels and the rigidity of CNCs. Meanwhile, the sponge gained superhydrophilic/underwater superhydrophobic wettability with an underwater oil contact angle of up to 165.7° due to its ordered micro/nanoscale structure. B-CNC sheets displayed high oil/water selectivity without additional material doping or chemical modification. For oil/water mixtures, high separation fluxes of approximately 100,000 L·m·h and separation efficiencies of up to 99.99 % were obtained. For a Tween 80-stabilized toluene-in-water emulsion, the flux reached >50,000 L·m·h, and the separation efficiency was above 99.7 %. B-CNC sponge sheets showed significantly higher fluxes and separation efficiencies than other bio-based two-dimensional materials. This research provides a facile and straightforward fabrication method of environmental-friendly B-CNC sponges for rapid, selective oil/water separation.