Ternary Heterostructure Membranes with Two-Dimensional Tunable Channels for Highly Selective Ion Separation

[Image: see text] Selective ion separation from brines is pivotal for attaining high-purity lithium, a critical nonrenewable resource. Conventional methods encounter substantial challenges, driving the quest for streamlined, efficient, and swift approaches. Here, we present a graphene oxide (GO)-based ternary heterostructure membrane with a unique design. By utilizing Zn(2+)-induced confinement synthesis in a two-dimensional (2D) space, we incorporated two-dimensional zeolitic imidazolate framework-8 (ZIF-8) and zinc alginate (ZA) polymers precisely within layers of the GO membrane, creating tunable interlayer channels with a ternary heterostructure. The pivotal design lies in ion insertion into the two-dimensional (2D) membrane layers, achieving meticulous modulation of layer spacing based on ion hydration radius. Notably, the ensuing layer spacing within the hybrid ionic intercalation membrane occupies an intermediary realm, positioned astutely between small-sized hydrated ionic intercalation membrane spacing and their more extensive counterparts. This deliberate configuration accelerates the swift passage of diminutive hydrated ions while simultaneously impeding the movement of bulkier ions within the brine medium. The outcome is remarkable selectivity, demonstrated by the partitioning of K(+)/Li(+) = 20.9, Na(+)/K(+) = 31.2, and Li(+)/Mg(2+) = 9.5 ion pairs. The ZIF-8/GO heterostructure significantly contributes to the selectivity, while the mechanical robustness and stability, improved by the ZA/GO heterostructure, further support its practical applicability. This report reports an advanced membrane design, offering promising prospects for lithium extraction and various ion separation processes.