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      Ultrathin graphene-based membrane with precise molecular sieving and ultrafast solvent permeation

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          Abstract

          Graphene oxide (GO) membranes continue to attract intense interest due to their unique molecular sieving properties combined with fast permeation rates. However, the membranes' use has been limited mostly to aqueous solutions because GO membranes appear to be impermeable to organic solvents, a phenomenon not fully understood yet. Here, we report efficient and fast filtration of organic solutions through GO laminates containing smooth two-dimensional (2D) capillaries made from flakes with large sizes of ~ 10-20 micron. Without sacrificing their sieving characteristics, such membranes can be made exceptionally thin, down to ~ 10 nm, which translates into fast permeation of not only water but also organic solvents. We attribute the organic solvent permeation and sieving properties of ultrathin GO laminates to the presence of randomly distributed pinholes that are interconnected by short graphene channels with a width of 1 nm. With increasing the membrane thickness, the organic solvent permeation rates decay exponentially but water continues to permeate fast, in agreement with previous reports. The application potential of our ultrathin laminates for organic-solvent nanofiltration is demonstrated by showing >99.9% rejection of various organic dyes with small molecular weights dissolved in methanol. Our work significantly expands possibilities for the use of GO membranes in purification, filtration and related technologies.

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          Most cited references31

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          MEMBRANE FILTRATION. Sub-10 nm polyamide nanofilms with ultrafast solvent transport for molecular separation.

          Membranes with unprecedented solvent permeance and high retention of dissolved solutes are needed to reduce the energy consumed by separations in organic liquids. We used controlled interfacial polymerization to form free-standing polyamide nanofilms less than 10 nanometers in thickness, and incorporated them as separating layers in composite membranes. Manipulation of nanofilm morphology by control of interfacial reaction conditions enabled the creation of smooth or crumpled textures; the nanofilms were sufficiently rigid that the crumpled textures could withstand pressurized filtration, resulting in increased permeable area. Composite membranes comprising crumpled nanofilms on alumina supports provided high retention of solutes, with acetonitrile permeances up to 112 liters per square meter per hour per bar. This is more than two orders of magnitude higher than permeances of commercially available membranes with equivalent solute retention.
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            Structural evolution during the reduction of chemically derived graphene oxide.

            The excellent electrical, optical and mechanical properties of graphene have driven the search to find methods for its large-scale production, but established procedures (such as mechanical exfoliation or chemical vapour deposition) are not ideal for the manufacture of processable graphene sheets. An alternative method is the reduction of graphene oxide, a material that shares the same atomically thin structural framework as graphene, but bears oxygen-containing functional groups. Here we use molecular dynamics simulations to study the atomistic structure of progressively reduced graphene oxide. The chemical changes of oxygen-containing functional groups on the annealing of graphene oxide are elucidated and the simulations reveal the formation of highly stable carbonyl and ether groups that hinder its complete reduction to graphene. The calculations are supported by infrared and X-ray photoelectron spectroscopy measurements. Finally, more effective reduction treatments to improve the reduction of graphene oxide are proposed.
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              Ultrathin Graphene Nanofiltration Membrane for Water Purification

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                Author and article information

                Journal
                15 September 2017
                Article
                1710.00047
                77bef529-371c-42a8-a5aa-4134110ecc43

                http://arxiv.org/licenses/nonexclusive-distrib/1.0/

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                Custom metadata
                physics.app-ph cond-mat.mtrl-sci physics.chem-ph

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