AbstractLithium extraction from salt lake brines is highly demanded to circumvent the lithium supply shortage. However, polymer nanofiltration membranes suffer from low lithium permeability while nanofluidic devices are hindered by complicated preparation and miniaturized scales despite high permeability. Here, the authors report a facile strategy to prepare positively charged nanofiltration membranes for ultrapermeable and selective separation of lithium ions from concentrated magnesium/lithium mixtures. A new electrolyte monomer (diaminoethimidazole bromide, DAIB) containing bidentate amine groups is designed to modify pristine polyamide composite membranes. Structure characterizations and simulations show that the DAIB modification brings about nano‐heterogeneity that not only improves surface hydrophilicity, but also reduces water transport resistance through the ≈100 nm thick separation layer. Water permeance of the modified membrane improves fivefold and is coupled with good stability in 200‐h continuous nanofiltration. It exhibits high lithium flux (0.7 mol m−2 h−1) for brines (Mg2+/Li+ ratio 20) at 6 bar operation pressure.
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