This research introduces highly efficient nanofiltration (NF) membranes designed for the effective rejection of both divalent cations and anions, a critical feature for advanced water treatment technologies. We have devised a simple yet adaptable approach for fabricating Janus polyamide (PA) thin-films characterized by dual charges, which exhibit pronounced selectivity towards both mono-/divalent anions and cations. Leveraging a straightforward interfacial polymerization (IP) process, we integrated high molecular weight polyethyleneimine (PEI) within the PA matrix. This strategy ensured the preferential formation of a dense, negatively charged upper layer dominated by piperazine (PIP), while cationic macromolecular PEI facilitated the emergence of a loose and positively charged lower layer, thus giving rise to a distinctively charged and structurally heterogeneous PA thin-film. Furthermore, the strategic inclusion of PEI inhibits the diffusion of the PIP, thereby promoting the development of nano-wrinkled structures. This structural innovation not only enhances pure water permeance (16.0 L m−2 h−1 bar−1) but also optimizes ion selectivity through the coordination of steric hindrance and Donnan effects. Consequently, the Janus charged NF membranes we developed exhibit exceptional selectivity for mono-/divalent ions, particularly demonstrating remarkable ion selectivity for Cl−/SO42− and Li+/Mg2+ of 102 and 24, respectively. Our findings introduce a pioneering avenue for fabricating NF membranes that proficiently separate mono-/divalent ions, promising significant advancements in water treatment and purification endeavors.
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