Mineralized Nanofiber Substrates Enabling High-Performance Dually Charged Nanofiltration Membranes with Enhanced Permeability

Nanofiltration membranes (NFMs) with superior permeability and high rejection of both divalent anions and cations are highly desirable to meet the increasing separation demands of complex systems. Herein, we propose a three-in-one strategy to develop a state-of-the-art dually charged thin-film composite (TFC) nanofiltration membrane consisting of a positively charged electrospun nanofiber substrate (NFS) with surface mineralization and a negatively charged polyamide (PA) selective layer prepared by interfacial polymerization (IP). The highly hydrophilic mineralized nanofiber substrate not only effectively reduces the thickness of the PA selective layer but also crumples its structures by the abundant zirconia nanoparticles on the substrate surface, resulting in excellent water flux (15.0 L m^-2 h^-1 bar^-1) for the TFC NFMs. The relationship between the thickness of the selective layer and substrate is further investigated using dissipative particle dynamics (DPD) simulations. Meanwhile, the dually charged NFM exhibits relatively high rejection for both anions (97.1% for Na₂SO₄ and 97.9% for MgSO₄) and cations (87.9% for MgCl₂) in aqueous solutions compared with single-charged membranes, which is attributed to the dual-repulsion effect of the selective layer and the substrate surface bearing opposite charges. Moreover, the prepared NFMs exhibit good stability and excellent antifouling performance. This work may pave the way for the development of highly efficient nanofiltration membranes for the practical separation of comprehensively charged solutes.