Tailoring Monovalent Ion Sieving in Graphene-Oxide Membranes with High Flux by Rationally Intercalating Crown Ethers

Two-dimensional membranes have shown promising potential for ion-selective separation due to their well-defined interlayer channels. However, the typical “trade-off” effect of throughput and selectivity limits their developments. Herein, we report a precise tailoring of monovalent cation sieving technology with enhanced water throughput via the intercalation of graphene-oxide membranes with selective crown ethers. By tuning the lamellar spacing of graphene oxide, a critical interlayer distance (∼11.04 Å) is revealed to maximize water flux (53.4 mol m –2 h –2 bar –1 ) without sacrificing ion selectivity. As a result, the elaborately enlarged interlayer distance offers improved water permeance. Meanwhile, various specific cations with remarkably high selectivity can be separated in mixed solutions because of the strong chelation with crown ethers. This work opens up a new avenue for high-throughput and precise regulation of ion separations for various application scenarios.