Membranes offer a scalable and cost-effective approach to ion separations for lithium recovery. In the case of salt-lake brines, however, the high feed salinity and low pH of the post-treated feed have an uncertain impact on nanofiltration's selectivity. Here, we adopt experimental and computational approaches to analyze the effect of pH and feed salinity and elucidate key selectivity mechanisms. Our data set comprises over 750 original ion rejection measurements, spanning five salinities and two pH levels, collected using brine solutions that model three salt-lake compositions. Our results demonstrate that the Li+/Mg2+ selectivity of polyamide membranes can be enhanced by 13 times with acid-pretreated feed solutions. This selectivity enhancement is attributed to the amplified Donnan potential from the ionization of carboxyl and amino moieties under low solution pH. As feed salinities increase from 10 to 250 g L-1, the Li+/Mg2+ selectivity decreases by ∼43%, a consequence of weakening exclusion mechanisms. Further, our analysis accentuates the importance of measuring separation factors using representative solution compositions to replicate the ion-transport behaviors with salt-lake brine. Consequently, our results reveal that predictions of ion rejection and Li+/Mg2+ separation factors can be improved by up to 80% when feed solutions with the appropriate Cl-/SO42- molar ratios are used.
Keywords: hypersaline brine; lithium extraction; nanofiltration; resource recovery; selectivity mechanism.