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. [Display omitted] •Metal-organic polyhedron-intercalated and crosslinked GO membranes are designed.•Uniformly distributed molecular cages refine vertical and interlayer pathways.•Membranes show good performance for removal of Na2SO4, dye, and antibiotic.•Membranes have great stability and sixfold permeance under cross-flow conditions.