Abstract
The remediation of emerging water contaminants, particularly per- and polyfluoroalkyl substances (PFAS), presents challenges due to their refractory nature and the presence of competing substances. Dual-functional adsorptive membranes, with hydrophobic backbone and quaternary ammonium moieties, were thereby designed to selectively intercept organic competitors while enrich PFAS. A 96.8% removal of perfluorooctanoic acid (PFOA) was achieved and this effective removal (>90%) maintained across five reuse cycles with a total treatment capacity of 650 L m(-2). Rather than the rejection mechanism of nanofiltration process, these adsorptive membranes utilize synergistic electrostatic attraction and hydrophobic interactions, leading to a greater enrichment factor of 18.5 (PFOA over humic acid) and a permeability of 34.6 L m(-2) h(-1) bar(-1) (1.9- and 4.5-fold higher than reported NF 270 membranes, respectively). Furthermore, computational fluid dynamics (CFD) modeling revealed that the sponge-like matrix effectively prevents channeling flow and enhance access to adsorption sites. Sensitivity analysis and the high Damkohler number indicated that the adsorption process is mass transfer-controlled, with the key parameters ranked in order of significance: residence time > fluid viscosity > intrinsic adsorption rate. With consistent removal performance with co-existing competitors, efficient regeneration, and reusability, the dual-functional adsorptive membranes offer promising practical efficacy for PFAS remediation.