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Two different types of 2D nanosheets, including hydrophobic graphene (GR) and hydrophilic graphene oxide (GO), were filled into poly (vinyl alcohol) (PVA) polymers to prepare mixed matrix membranes (MMMs) for ethanol dehydration via pervaporation. The relationship between the physical/chemical properties of graphene and pervaporation performance of MMMs was investigated by a comparison of GR/PVA and GO/PVA MMMs in microstructure and PV performance. The incorporation of GO nanosheets into PVA reduced PVA crystallinity and enhanced the membrane hydrophilicity, while the incorporation of GR into PVA led to the opposite results. The incorporation of GR/GO into PVA depressed the PVA membrane swelling degree, and the incorporation of GR showed a more obvious depression effect. GR/PVA MMMs showed a much higher separation factor than GO/PVA MMMs, while they exhibited a much lower permeation flux than GO/PVA MMMs and pristine PVA membranes. The huge difference in microstructure and performance between GO/PVA and GR/PVA MMMs was strongly associated with the oxygen-containing groups on graphene lamellae. The higher permeation flux of GO/PVA MMMs was ascribed to the facilitated transport of water molecules induced by oxygen-containing groups and exclusive channels provided by GO lamellae, while the much lower permeation flux and higher separation factor GR/PVA MMMs was resulted from the smaller GR interplanar spacing (0.33 nm) and hydrophobicity as well as barrier effect of GR lamellae on the sorption and diffusion of water molecules. It was presumed that graphene intercalated with an appropriate number of oxygen-containing groups might be a good choice to prepare PVA-based MMMs for ethanol dehydration, which would combine the advantages of GR’s high interlayer diffusion selectivity and GO’s high permeation properties. The investigation might open a door to achieve both of high permeation flux and separation factor of PVA-based MMMs by tuning the microstructure of graphene.

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Graphene oxide (GO), owing to its atomic thickness and tunable physicochemical properties, exhibits fascinating properties in membrane separation fields, especially in water treatment applications (due to unimpeded permeation of water through graphene-based membranes). Particularly, GO-based membranes used for desalination via pervaporation or nanofiltration have been widely investigated with respect to membrane design and preparation. However, the precise construction of transport pathways, facile fabrication of large-area GO-based membranes (GOMs), and robust stability in desalination applications are the main challenges restricting the industrial application of GOMs. This review summarizes the challenges and recent research and development of GOMs with respect to preparation methods, the regulation of GOM mass transfer pathways, desalination performance, and mass transport mechanisms. The review aims to provide an overview of the precise regulation methods of the horizontal and longitudinal mass transfer channels of GOMs, including GO reduction, interlayer cross-linking, intercalation with cations, polymers, or inorganic particles, etc., to clarify the relationship between the microstructure and desalination performance, which may provide some new insight regarding the structural design of high-performance GOMs. Based on the above analysis, the future and development of GOMs are proposed.