Ionic liquid-induced deep grafting of polyelectrolyte to reform polyamide layer for antifouling nanofiltration membrane

Surface grafting has been widely used to tune hydrophilicity and chargeability of nanofiltration membranes for reducing membrane fouling potential. However, surface grafting typically leads to a significant pore narrowing and resultant permeability loss, and monocharged surface still struggles to resist mixed foulants with different charges. Herein, ionic liquid (IL)-ethanol (EtOH) solution containing polyethyleneimine (PEI) is used to rearrange the nascent polyamide layer. The high affinity of IL to the PA layer and the low diffusion steric hindrance of EtOH contribute to the polyamide swelling and PEI deep grafting, during which the "self-regulation" effect (larger pores would be filled with more PEI molecules) narrows the pore size distribution and enhances hydrophilicity. The nearly charge-neutral and smooth separation layer shows impressive antifouling capacity to hydrophobic macromolecules and mixed charged molecules, along with long-term operating stability for real wastewater treatment. This study emphasizes the importance of solvent properties on the membrane grafting behavior.