Self-assembly of stable and high-performance molecular cage-crosslinked graphene oxide membranes for contaminant removal

Membrane separation is regarded as efficient technology to alleviate global water crisis. Two-dimensional membranes are promising for contaminant removal from wastewaters, but their uncontrollable transport pathway and instability hinder the further development. In this study, the high-performance and stable two-dimensional framework membranes are self-assembled by graphene oxide (GO) nanosheets and amino-appended metal-organic polyhedrons (MOPs) for water purification and remediation. The MOP molecular cages are uniformly intercalated between GO nanosheets and enriched at defects/edges, and can crosslink membranes, to provide in-plane selective channels, refine vertical passageways, and fix out-of-plane interlayer spaces. The prepared GO/MOP framework membranes have improved stability and nanofiltration performance under cross-flow condition, can keep performance in water after 50 h filtration, and show high rejections over 92% for Na2SO4 and 99% for antibiotic and dye contaminants with molecular weights over 280 g mol-1, and sixfold permeance as that of GO membranes. Our molecular cage-intercalated and crosslinked two-dimensional frameworks offer an alternative route to design robust membranes for efficient removal of contaminants in wastewaters.