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Recent Developments of Graphene Oxide-Based Membranes: a Review membranes Review Recent Developments of Graphene Oxide-Based Membranes: A Review Jinxia Ma, Dan Ping and Xinfa Dong * School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510641, China; [email protected] (J.M.); [email protected] (D.P.) * Correspondence: [email protected]; Tel./Fax: +86-020-8711-0659 Received: 3 July 2017; Accepted: 3 September 2017; Published: 12 September 2017 Abstract: Membrane-based separation technology has attracted great interest in many separation fields due to its advantages of easy-operation, energy-efficiency, easy scale-up, and environmental friendliness. The development of novel membrane materials and membrane structures is an urgent demand to promote membrane-based separation technology. Graphene oxide (GO), as an emerging star nano-building material, has showed great potential in the membrane-based separation field. In this review paper, the latest research progress in GO-based membranes focused on adjusting membrane structure and enhancing their mechanical strength as well as structural stability in aqueous environment is highlighted and discussed in detail. First, we briefly reviewed the preparation and characterization of GO. Then, the preparation method, characterization, and type of GO-based membrane are summarized. Finally, the advancements of GO-based membrane in adjusting membrane structure and enhancing their mechanical strength, as well as structural stability in aqueous environment, are particularly discussed. This review hopefully provides a new avenue for the innovative developments of GO-based membrane in various membrane applications. Keywords: membrane; graphene oxide; graphene oxide membrane; separation performance; structural stability 1. Introduction In the past few decades, membrane-based separation technology has attracted considerable attention in many separation fields due to its advantages of easy-operation, energy-efficiency, and environmental friendliness [1]. Advanced membranes with superior selectivity and permeability are essential to the development of membrane-based separation technology. Currently, polymeric membrane has governed the entire membrane market, including real-world application and academic research, owing to its advantages of energy-efficiency, easy-operation, low-cost, and inherent simplicity. Nevertheless, restrictions of polymeric membranes still exist for most practical applications, because most of them tend to foul, have low resistance to chlorine, strong acids/alkaline, high temperature and organic solvents, and suffer from aperture shrinkage under high pressure [2]. The strong trade-off relation between membrane selectivity and permeability is a common challenge for all of polymeric membranes [3]. These restrictions have urged membrane scientists to constantly seek new membrane materials and develop novel membrane structures with superior chemical stability, thermal stability, water permeability, as well as high selectivity [4]. Recently, carbon-based materials like carbon nanotubes (CNTs), graphene, and its derivative graphene oxide (GO), have shown notable potential in membrane-based separation fields because of their strong mechanical strength, high resistance to strong acids/alkaline and organic solvents, and easy accessibility [5–8]. Among them, GO was served as one of the emerging nano-building materials for the fabrication of novel separation membrane owing to its distinct two-dimensional (2D) and single-atomic-thick structure, high mechanical strength, Membranes 2017, 7, 52; doi:10.3390/membranes7030052 www.mdpi.com/journal/membranes Membranes 2017, 7, 52 2 of 29 Membranes 2017, 7, 52 2 of 29 frictionless surface, and good flexibility combined with large-scale and cost-effective production in highsolution chemical [9–11]. inertness, nearly frictionless surface, and good flexibility combined with large-scale and cost-effectiveGO was production first synthesized in solution by [9– 11Brodie]. [12] in 1859. Subsequently, Staudenmaier [13] and HummersGO was [14] first improved synthesized the preparation by Brodie method [12] in in 1859. 1898 and Subsequently, 1958, respectively. Staudenmaier Afterwards, [13] several and Hummersmodified [14 Hummers’] improved methods the preparation as well methodas some in other 1898 andnew 1958, methods respectively. were successively Afterwards, developed several modified[15–17]. Hummers’ In order to methods identify as the well surface as some morpho other newlogy methods and chemical were successively structure of developed the resultant [15–17 GO,]. Inseveral order tocharacterization identify the surface techniques morphology are widely and em chemicalployed, structuresuch as atomic of the force resultant microscopy GO, several (AFM), characterizationscanning electron techniques microscopy are widely (SEM), employed, transmission such aselectron atomic microscopy force microscopy (TEM), (AFM), X-ray scanningdiffraction electron(XRD), microscopy Raman spectroscopy, (SEM), transmission X-ray photoelectron electron microscopy spectroscopy (TEM), (XPS), X-ray diffractionFourier-transform (XRD), Raman infrared spectroscopy,spectroscopy X-ray (FTIR), photoelectron thermogravimetric spectroscopy analysis (XPS), Fourier-transform(TGA), and Zeta infrared potential spectroscopy [15,16,18,19]. (FTIR), The thermogravimetricresultant GO contains analysis plentiful (TGA), andof oxygenated Zeta potential functional [15,16,18, 19groups—such]. The resultant as GOhydroxyl, contains epoxy, plentiful and ofcarboxyl—on oxygenated functional its basal plane groups—such and at its as edge hydroxyl, [20], as epoxy, shown and in carboxyl—onFigure 1. These its basalfunctional plane groups and atendow its edge GO [20 ],good as shown hydrophilicity in Figure1 and. These favorable functional water groups solubility, endow which GO good enables hydrophilicity a convenient and and favorablecost-effective water solution solubility, process which for enables the preparat a conveniention of andGO-based cost-effective membrane solution [21,22]. process Additionally, for the preparationthese oxygenated of GO-based functional membrane groups [21 make,22]. Additionally,GO nanosheets these readily oxygenated to be further functional surface-modified groups make and GOthe nanosheets correspondingly readily to functional be further surface-modifiedGO-based comp andosite the membranes correspondingly with functionalpreferable GO-based separation compositeperformance membranes can be obtained. with preferable separation performance can be obtained. FigureFigure 1. Structure 1. Structure mode mode of graphene of graphene oxide oxide [23]. Copyrigh [23]. Copyrightt 2015 Journal 2015 Journal of the Physical of the Physical Society Societyof Japan. of Japan. Based on these advantages as well as high surface-to-volume ratio structure of GO nanosheets, variousBased GO-based on these advantages membranes as have well been as high widely surface-to-volume developed and ratio exhibited structure great of GOpromise nanosheets, in many variousmembrane GO-based separation membranes fields such have as been gas separation widely developed [24,25], water and exhibited purification great [26], promise desalination in many [27], membraneand pervaporation separation (PV) fields [28]. such In asrecent gas separation decades, patents [24,25], and water papers purification (including [26 ],research desalination articles [27 and], andreview pervaporation papers) focusing (PV) [28 on]. InGO-based recent decades, membranes patents are andgrowing papers exponentially, (including research as shown articles in Figure and 2. reviewAmong papers) them, focusing several on review GO-based papers membranes focused areon growingsummarizing exponentially, the structure, as shown physicochemical in Figure2. Amongproperty, them, application, several review and papers separation focused mechanism on summarizing of GO-based the structure, membranes physicochemical appeared [9,23,29–39]. property, application,Based on these and separation research articles, mechanism we le ofarned GO-based that the membranes structure, mechanical appeared [9 strength,,23,29–39 and]. Based structural on thesestability research of GO-based articles, we membrane learned that have the significant structure, influence mechanical on membrane strength, and separation structural performance. stability of GO-basedIn membranethis review have paper, significant the latest influence research on membraneprogress in separation GO-based performance. membranes centered on improvingIn this reviewmembrane paper, structure, the latest mechanical research strength progress as in well GO-based as structural membranes stability centered in aqueous on improvingsolution is membrane highlighted structure, and discussed mechanical in more strength detail. First, as well we asbriefly structural reviewed stability the preparation in aqueous and solutioncharacterization is highlighted of GO. and Then, discussed the preparation in more detail. method, First, characterization, we briefly reviewed and type the preparationof GO-based andmembrane characterization are summarized. of GO. Then, Finally, the preparation the advanc method,ements characterization, of GO-based membrane and type of in GO-based adjusting membranemembrane are structure summarized. and enhancing Finally, thetheir advancements mechanical strength of GO-based as well membrane as structural in adjustingstability in membraneaqueous structureenvironment and enhancingare particularly their mechanicaldiscussed,
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