Shearing Liquid‐Crystalline MXene into Lamellar Membranes with Super‐Aligned Nanochannels for Ion Sieving

Abstract Ion‐selective membranes are crucial in various chemical and physiological processes. Numerous studies have demonstrated progress in separating monovalent/multivalent ions, but efficient monovalent/monovalent ion sieving remains a great challenge due to their same valence and similar radii. Here, this work reports a two‐dimensional (2D) MXene membrane with super‐aligned slit‐shaped nanochannels with ultrahigh monovalent ion selectivity. The MXene membrane is prepared by applying shear forces to a liquid‐crystalline (LC) MXene dispersion, which is conducive to the highly‐ordered stacking of the MXene nanosheets. The obtained LC MXene membrane (LCMM) exhibits ultrahigh selectivities toward Li + /Na + , Li + /K + , and Li + /Rb + separation (≈45, ≈49, and ≈59), combined with a fast Li + transport with a permeation rate of ≈0.35 mol m −2 h −1 , outperforming the state‐of‐the‐art membranes. Theoretical calculations indicate that in MXene nanochannels, the hydrated Li + with a tetrahedral shape has the smallest diameter among the monovalent ions, contributing to the highest mobility. Besides, the weakest interaction is found between hydrated Li + and MXene channels which also contributes to the ultrafast permeation of Li + through the super‐aligned MXene channels. This work demonstrates the capability of MXene membranes in monovalent ion separation, which also provides a facile and general strategy to fabricate lamellar membranes in a large scale.