The surface properties and microstructure of graphene oxide (GO)-based membranes are both crucial for enhanced nanofiltration performance. Herein, a GO nanofiltration membrane is fabricated with regulatable surface properties and microstructure via a facile two-step impregnation in KOH and following HCl aqueous solutions. The type and number of oxygen-containing groups in GO membranes change with fewer C-O-C/C-OH and C═O but more COOH groups, and they are readily regulated by alkaline treatment time, which enables enhanced surface hydrophilicity and larger surface ζ potentials. Meanwhile, a few tiny defects are present in the GO sheets, which could increase the number of pores and decrease the length of water nanochannels. Such surface properties and microstructure together determine the excellent nanofiltration performance of the GO membranes with fast and selective water permeation, e.g., ∼99.5% rejection toward CBB G250 and flux of 56.9 ± 1.0 L m-2 h-1. This work provides insights into the design of high-performance two-dimensional laminar membranes.
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