We introduce a novel and facile approach to improve the desalination performance of pressure-driven layer-by-layer (LbL) assembled membranes. Electrostatic LbL multilayers composed of weak polyelectrolytes (PEs), e.g., cationic poly(allylamine hydrochloride) (PAH) and anionic poly(acrylic acid) (PAA), were prepared on commercial polysulfone substrates. In order to measure the ion rejection and permeate flux of these membranes, the ionic concentration of the feed solution and operating pressure were fixed at 2000 ppm NaCl and 20 bar, respectively. It was observed that the crosslinked (PAH pH 7.5/PAA pH 3.5)n=10,20 multilayers, which were assembled at the pH conditions allowing a low charge density of the respective PEs, show relatively high ion rejection compared to other multilayers. This result suggests that the optimal structures for desalination membranes should contain a large amount of freely charged groups with densely-packed structures via crosslinking. Finally, the recycling process was employed to further improve the desalination performance. In this case the (PAH pH 7.5/PAA pH 3.5)n=10,20 multilayers exhibited the ion rejection up to 99.8%. This pH-controlled and thermal crosslinking method suggests a new route for the design of well-defined desalination reverse osmosis membranes based on LbL multilayers.
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