Enhanced Mono/Divalent Ion Separation via Charged Interlayer Channels in Montmorillonite-Based Membranes

Efficient mono- and divalent ion separation is pivotal for environmental conservation and energy utilization. Two-dimensional (2D) materials featuring interlayer nanochannels exhibit unique water and ion transport properties, rendering them highly suitable for water treatment membranes. In this work, we incorporated polydopamine/polyethylenimine (PDA/PEI) copolymers into 2D montmorillonite (MMT) nanosheet interlayer channels through electrostatic interactions and bioinspired bonding. A modified laminar structure was formed on the substrate surface via a straightforward vacuum filtration. The electrodialysis experiments reveal that these membranes could achieve monovalent permselectivity of 11.06 and Na⁺ flux of 2.09 × 10^-8 mol cm^-2 s^-1. The enhanced permselectivity results from the synergistic effect of electrostatic and steric hindrance effect. In addition, the interaction between the PDA/PEI copolymer and the MMT nanosheet ensures the long-term operational stability of the membranes. Theoretical simulations reveal that Na⁺ has a lower migration energy barrier and higher migration rate for the modified MMT-based membrane compared to Mg²⁺. This work presents a novel approach for the development of monovalent permselective membranes.