界面自组装法制备高性能氧化石墨烯膜
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摘要
为制备可靠、精确的分子筛氧化石墨烯(GO)膜,克服基于厚度调控的抽滤自组装GO膜分离性能提升和通量减小之间的矛盾关系,采用界面自组装法,制备了具有更加紧密层间结构的GO膜,并对其性能进行了表征。实验结果表明:与抽滤自组装法制备GO膜相比,界面自组装法可以实现更加紧密的层间结构;在化学环境相似的条件下,界面自组装膜的层间距可达0.75 nm,较抽滤自组装膜减小了0.10 nm左右;成膜机理和速率是GO膜层间结构的主要影响因素。将该膜用于金属离子水溶液的截留实验,结果表明:界面自组装GO膜对Mg~(2+)的截留率可达70%左右,是抽滤自组装膜的1.3倍。
To prepare reliable and accurate graphene oxide(GO) membrane for molecular sieving, the interface self-assembly method is adopted to prepare GO membranes with more compact interlayer structure. This method can solve the problem that the contradictory relationship between the separation performance and flux caused by thickness control when tuning the performance of GO membrane. The experimental results showed that the interface self-assembly method can achieve closer interlayer structure compared with filtration self-assembly. Under the condition of similar chemical environment, the interlayer spacing can reach about 0.75 nm, which is reduced0.10 nm than that of filtration self-assembly GO membrane. The formation mechanism and rate are the main factors influencing the interlayer structure. The desalting experiment of the membrane for metallic cations/water solution showed that the rejection rate of the interface self-assembled GO membrane for Mg~(2+) was about 70%,which was 1.3 times of the self-assembly membrane.
To prepare reliable and accurate graphene oxide(GO) membrane for molecular sieving, the interface self-assembly method is adopted to prepare GO membranes with more compact interlayer structure. This method can solve the problem that the contradictory relationship between the separation performance and flux caused by thickness control when tuning the performance of GO membrane. The experimental results showed that the interface self-assembly method can achieve closer interlayer structure compared with filtration self-assembly. Under the condition of similar chemical environment, the interlayer spacing can reach about 0.75 nm, which is reduced0.10 nm than that of filtration self-assembly GO membrane. The formation mechanism and rate are the main factors influencing the interlayer structure. The desalting experiment of the membrane for metallic cations/water solution showed that the rejection rate of the interface self-assembled GO membrane for Mg~(2+) was about 70%,which was 1.3 times of the self-assembly membrane.
引文
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[3]GOH K,SETIAWAN L,WEI L,et al.Graphene oxide as effective selective barriers on a hollow fiber membrane for water treatment process[J].Journal of Membrane Science,2015,474:244-253.
[4]SHEN J,ZHANG M,LIU G,et al.Facile tailoring of the twodimensional graphene oxide channels for gas separation[J].RSCAdvances,2016,6(59):54281-54285.
[5]KIM H W,YOON H W,YOON S M,et al.Selective gas transport through few-layered graphene and graphene oxide membranes[J].Science,2013,342(6154):91-95.
[6]HU M,MI B.Enabling graphene oxide nanosheets as water separation membranes[J].Environmental Science&Technology,2013,47(8):3715-3723.
[7]FENG B,XU K,HUANG A.Covalent synthesis of three-dimensional graphene oxide framework(GOF)membrane for seawater desalination[J].Desalination,2016,394:123-130.
[8]WERBER J R,OSUJI C O,ELIMELECH M.Materials for next-generation desalination and water purification membranes[J].Nature Reviews Materials,2016(5):16018-16032.
[9]HUNG W S,TSOU C H,GUZMAN M D,et al.Cross-linking with diamine monomers to prepare composite graphene oxideframework membranes with varying d-spacing[J].Chemistry of Materials,2014,26(9):2983-2990.
[10]CHEN L,SHI G,SHEN J,et al.Ion sieving in graphene oxide membranes via cationic control of interlayer spacing[J].Nature,2017,550(7676):380-383.
[11]LIU H,WANG H,ZHANG X.Facile fabrication of freestanding ultrathin reduced graphene oxide membranes for water purification[J].Advanced Materials,2015,27(2):249-254.
[12]MENG N,ZHAO W,SHAMSAEI E,et al.A low-pressure GO nanofiltration membrane crosslinked via Ethylenediamine[J].Journal of Membrane Science,2017,548:363-371.
[13]HUANG H,SONG Z,WEI N,et al.Ultrafast viscous water flow through nanostrand-channelled graphene oxide membranes[J].Nature Communications,2013,4(4):2979-2988.
[14]HAN Y,JIANG Y,GAO C.High-flux graphene oxide nanofiltration membrane intercalated by carbon nanotubes[J].ACS Applied Material and Interfaces,2015,7(15):8147-8155.
[15]ABRAHAM J,VASU K S,WILLIAMS C D,et al.Tunable sieving of ions using graphene oxide membranes[J].Nature Nanotechnology,2017,12(6):546-550.
[16]XU W L,FANG C,ZHOU F,et al.Self-assembly:A facile way of forming ultrathin,high-performance graphene oxide membranes for water purification[J].Nano Letters,2017,17(5):2928-2933.
[17]魏伟,吕伟,杨全红.高浓度石墨烯水系分散液及其气液界面自组装膜[J].新型炭材料,2011,26(1):36-40.WEI W,LYU W,YANG Q H.High-concentratiom graphene aquous suspension and a membrane self-assembled at the liquid-air interface[J].New Carbon Materials,2011,26(1):36-40(in Chinese).
[18]CHEN D,FENG H,LI J.Graphene oxide:Preparation,functionalization,and electrochemical applications[J].Chemical Reviews,2012,112(11):6027-6053.
[19]MARCANO D C,KOSYNKIN D V,BELIN J M,et al.Improved synthesis of graphene oxide[J].ACS Nano,2010,4(8):4806-4814.
[20]YANG D,VELAMAKANNI A,BOZOKLU G,et al.Chemical analysis of graphene oxide films after heat and chemical treatments by X-ray photoelectron and micro-Raman spectroscopy[J].Carbon,2009,47(1):145-152.
[21]BLANTON T N,MAJUMDAR D.Characterization of X-ray irradiated graphene oxide coatings using X-ray diffraction,X-ray photoelectron spectroscopy,and atomic force microscopy[J].Powder Diffraction,2013,28(2):68-71.