Efficient Mg2+ and Li+ separation is a critical challenge in lithium recovery from brines because Mg2+ is typically abundant and has a hydrated radius comparable to that of Li+, creating a highly competitive ionic environment. Here, we consider a binary MgCl2/LiCl solution and employ molecular dynamics (MD) simulations to investigate how the feed-side magnesium to lithium (Mg/Li) ratio modulates Mg2+ and Li+ transport through an ideal single-layer neutral ZIF-8 membrane. The MD simulations were performed under accelerated hydraulic driving pressure to quantify Li+ flux, purity, enrichment factor, and separation factor for different Mg/Li ratios. Within the accelerated-pressure range investigated, 750 MPa provides the best balance between Li+ permeation and Mg2+ exclusion. At this pressure, an Mg/Li ratio of 1 yields the highest separation and enrichment factors among all feed compositions examined. Restrained potential-energy calculations show that Mg2+ encounters a higher energetic resistance to pore entry than Li+. Consequently Mg2+ accumulation near the pore entrance restricted Li+ access as the feed Mg/Li ratio increased, whereas higher pressures promoted Mg2+ permeation and reduced separation performance. A MACE potential fine-tuned with DFT further revealed broader pore accessibility for Li+, while the DFT calculations confirmed the stronger Mg2+-water interaction. These findings provide molecular-level mechanistic insight into composition-dependent Mg2+ and Li+ transport in ideal ZIF-8 nanopores.


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