Enhanced adsorption of uranium (VI) using a three-dimensional layered double hydroxide/graphene hybrid material

Abstract This study presents a facile route for the fabrication of a hierarchical three-dimensional composite (layered double hydroxide/graphene). The composite was obtained via in situ growth of layered double hydroxide (LDH) nanosheet arrays onto graphene sheets. The materials were characterized by transmission electron microscopy, scanning electron microscope, Fourier-transform infrared spectroscopy, X-ray diffraction and Brunauer–Emmett–Teller surface area measurement. This particularly structured composite has a large specific surface area and typical mesoporous characteristics, which are favorable for achieving high adsorption performance. The influence of conditions for uranium adsorption, including pH of aqueous solution, adsorbent dose, shaking time, and temperature were investigated. The results reveal that the maximum adsorption capacity of the layered double hydroxide/graphene toward uranium (VI) is 277.80 mg g−1, displaying a high efficiency for the removal of uranium (VI) from aqueous solution. The thermodynamic parameters, such as ΔH°, ΔS°, and ΔG° show that the process is endothermic and spontaneous. The kinetic adsorption can be described by a pseudo-second-order rate equation. This work describes an efficient, fast, and convenient approach for the removal of uranium (VI) from aqueous solutions.

[1]  Lili Zhang,et al.  Facile synthesis of NiAl-layered double hydroxide/graphene hybrid with enhanced electrochemical properties for detection of dopamine. , 2011, Nanoscale.

[2]  C. K. Gupta,et al.  Uranium Resource Processing: Secondary Resources , 2003 .

[3]  Jun Wang,et al.  In situ grown of nano-hydroxyapatite on magnetic CaAl-layered double hydroxides and its application in uranium removal , 2012 .

[4]  A. Cirelli,et al.  Cr(VI) and Cr(III) removal from aqueous solution by raw and modified lignocellulosic materials: a review. , 2010, Journal of hazardous materials.

[5]  Hua Zhang,et al.  Graphene‐Based Electrodes , 2012, Advanced materials.

[6]  Amit Bhatnagar,et al.  A comparative adsorption study with different industrial wastes as adsorbents for the removal of cationic dyes from water. , 2005, Journal of colloid and interface science.

[7]  Bo Gao,et al.  Enhanced high-current capacitive behavior of graphene/CoAl-layered double hydroxide composites as electrode material for supercapacitors , 2012 .

[8]  R. Cattrall,et al.  Extraction of uranium(VI) from sulfate solutions using a polymer inclusion membrane containing di-(2-ethylhexyl) phosphoric acid , 2010 .

[9]  H. Zänker,et al.  Aqueous suspensions of carbon nanotubes: surface oxidation, colloidal stability and uranium sorption. , 2009, Environmental pollution.

[10]  Xiangke Wang,et al.  A brief review of graphene-based material synthesis and its application in environmental pollution management , 2012 .

[11]  Shunsuke Tanaka,et al.  Theoretical analysis of the pseudo-second order kinetic model of adsorption. Application to the adsorption of Ag(I) to mesoporous silica microspheres functionalized with thiol groups , 2013 .

[12]  Qianqian Li,et al.  Microwave-assisted synthesis of CoAl-layered double hydroxide/graphene oxide composite and its application in supercapacitors , 2012 .

[13]  D. E. Bryant,et al.  Development of a functionalized polymer-coated silica for the removal of uranium from groundwater. , 2003, Environmental science & technology.

[14]  A. Zouboulis,et al.  Removal of metal Ions from dilute aqueous solutions: A comparative study of inorganic sorbent materials , 1999 .

[15]  A. Omer.  Energy, environment and sustainable development , 2008 .

[16]  Klaus Müllen,et al.  Composites of Graphene with Large Aromatic Molecules , 2009 .

[17]  Feng Li,et al.  Anchoring Hydrous RuO2 on Graphene Sheets for High‐Performance Electrochemical Capacitors , 2010 .

[18]  Inyoung Kim,et al.  Self-assembly of layered double hydroxide 2D nanoplates with graphene nanosheets: an effective way to improve the photocatalytic activity of 2D nanostructured materials for visible light-induced O2 generation , 2013 .

[19]  Gordon McKay,et al.  The kinetics of sorption of divalent metal ions onto sphagnum moss peat , 2000 .

[20]  Bernadette A. Hernandez-Sanchez,et al.  Synthesis and Characterization of Titania-Graphene Nanocomposites. , 2009 .

[21]  W. Daud,et al.  Removal of Hexavalent Chromium-Contaminated Water and Wastewater: A Review , 2009 .

[22]  R. Mark Bricka,et al.  A review of potentially low-cost sorbents for heavy metals , 1999 .

[23]  M. Osada,et al.  Synthesis, anion exchange, and delamination of Co-Al layered double hydroxide: assembly of the exfoliated nanosheet/polyanion composite films and magneto-optical studies. , 2006, Journal of the American Chemical Society.

[24]  Xiaojing Yang,et al.  Intercalation of Organic Ammonium Ions into Layered Graphite Oxide , 2002 .

[25]  Min Wei,et al.  Hierarchical films of layered double hydroxides by using a sol-gel process and their high adaptability in water treatment. , 2010, Chemical communications.

[26]  Yi Xie,et al.  Ultrathin two-dimensional MnO2/graphene hybrid nanostructures for high-performance, flexible planar supercapacitors. , 2013, Nano letters.

[27]  Guanghui Wang,et al.  Adsorption of uranium (VI) from aqueous solution onto cross-linked chitosan. , 2009, Journal of hazardous materials.

[28]  Jun Wang,et al.  Synthesis of aluminananosheetsvia supercritical fluid technology with high uranyl adsorptive capacity , 2013 .

[29]  C. A. Morais,et al.  Uranium stripping from tertiary amine loaded solution by ammonium sulfate , 2005 .

[30]  K. Dash,et al.  Synergistic Extraction of Uranium(VI) by Mixtures of β-Diketones and Structurally Related Crown Ethers , 1998 .

[31]  Ibrahim Dincer,et al.  Exergy: Energy, Environment and Sustainable Development , 2007 .

[32]  M. Rajamathi,et al.  Graphene–nanocrystalline metal sulphide composites produced by a one-pot reaction starting from graphite oxide , 2009 .

[33]  M. Antony,et al.  Extraction of uranium by amine, amide and benzamide grafted covalently on silica gel , 2004 .

[34]  J. Schaller,et al.  Effects of gamma-sterilization on DOC, uranium and arsenic remobilization from organic and microbial rich stream sediments. , 2011, The Science of the total environment.

[35]  C. A. Morais,et al.  Thorium and uranium extraction from rare earth elements in monazite sulfuric acid liquor through solvent extraction , 2010 .

[36]  Jiaxing Li,et al.  Synthesis of amidoxime-functionalized Fe3O4@SiO2 core–shell magnetic microspheres for highly efficient sorption of U(VI) , 2014 .

[37]  Gan Tian,et al.  Sorption of uranium(VI) using oxime-grafted ordered mesoporous carbon CMK-5. , 2011, Journal of hazardous materials.

[38]  I. Langmuir.  THE ADSORPTION OF GASES ON PLANE SURFACES OF GLASS, MICA AND PLATINUM. , 1918 .

[39]  Hendrik Ulbricht,et al.  Interlayer cohesive energy of graphite from thermal desorption of polyaromatic hydrocarbons , 2004 .

[40]  Tao Wen,et al.  Preconcentration of U(VI) ions on few-layered graphene oxide nanosheets from aqueous solutions. , 2012, Dalton transactions.

[41]  Min Wei,et al.  Erasable nanoporous antireflection coatings based on the reconstruction effect of layered double hydroxides. , 2010, Angewandte Chemie.

[42]  Jianfu Zhao,et al.  Enhanced adsorption of acid brown 14 dye on calcined Mg/Fe layered double hydroxide with memory effect , 2013 .

[43]  David Chadwick,et al.  Graphene Oxide as Support for Layered Double Hydroxides: Enhancing the CO2 Adsorption Capacity , 2012 .

[44]  H. Dai,et al.  Ni(OH)2 nanoplates grown on graphene as advanced electrochemical pseudocapacitor materials. , 2010, Journal of the American Chemical Society.

[45]  Hui Wang,et al.  Facile synthesis and novel electrocatalytic performance of nanostructured Ni–Al layered double hydroxide/carbon nanotube composites , 2010 .

[46]  H. Freundlich.  Über die Adsorption in Lösungen , 1907 .

[47]  Yan Gao,et al.  Individual and competitive adsorption of phosphate and arsenate on goethite in artificial seawater , 2003 .

[48]  Chaohui He,et al.  Synthesis and application of magnetic graphene/iron oxides composite for the removal of U(VI) from aqueous solutions , 2013 .

[49]  Xiaodong Wu,et al.  Synthesis of amphiphilic graphite oxide , 2008 .

[50]  Kian Ping Loh,et al.  The chemistry of graphene , 2010 .