Journal Home > Volume 4 , Issue 6
Nano Research 2011, 4(6): 550-562 https://doi.org/10.1007/s12274-011-0111-3
Research Article | Issue | Published: 18 February 2011

Magnetite/Reduced Graphene Oxide Nanocomposites: One Step Solvothermal Synthesis and Use as a Novel Platform for Removal of Dye Pollutants

Show Author's Information Hongmei Sun1,2,  Linyuan Cao1,2,  Lehui Lu1( )
State Key Laboratory of Electroanalytical ChemistryChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022China
Graduate School of the Chinese Academy of SciencesBeijing100039China
Keywords:
nanocomposites, graphene, Magnetic nanoparticles, removal, dye pollutants
Cite this article:
Sun H, Cao L, Lu L. Magnetite/Reduced Graphene Oxide Nanocomposites: One Step Solvothermal Synthesis and Use as a Novel Platform for Removal of Dye Pollutants. Nano Research, 2011, 4(6): 550-562. https://doi.org/10.1007/s12274-011-0111-3
Download citation
EndNote(RIS)
BibTeX

662

Views

38

Downloads

Citations

571

Crossref

N/A

WoS

604

Scopus

21

CSCD

Abstract Full text Electronic supplementary material About this article

A simple one step solvothermal strategy using non-toxic and cost-effective precursors has been developed to prepare magnetite/reduced graphene oxide (MRGO) nanocomposites for removal of dye pollutants. Taking advantage of the combined benefits of graphene and magnetic nanoparticles, these MRGO nanocomposites exhibit excellent removal efficiency (over 91% for rhodamine B and over 94% for malachite green) and rapid separation from aqueous solution by an external magnetic field. Interestingly, the performance of the MRGO composites is strongly dependent on both the loading of Fe3O4 and the pH value. In addition, the adsorption behavior of this new adsorbent fits well with the Freundlich isotherm and the pseudo-second-order kinetic model. In further applications, real samples—including industrial waste water and lake water—have been treated using the MRGO composites. All the results demonstrate that the MRGO composites are effective adsorbents for removal of dye pollutants and thus could provide a new platform for dye decontamination.


menu
Abstract
Full text
Outline
Electronic supplementary material
About this article

Magnetite/Reduced Graphene Oxide Nanocomposites: One Step Solvothermal Synthesis and Use as a Novel Platform for Removal of Dye Pollutants

Show Author's information Hongmei Sun1,2, Linyuan Cao1,2, Lehui Lu1( )
State Key Laboratory of Electroanalytical ChemistryChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022China
Graduate School of the Chinese Academy of SciencesBeijing100039China

Abstract

A simple one step solvothermal strategy using non-toxic and cost-effective precursors has been developed to prepare magnetite/reduced graphene oxide (MRGO) nanocomposites for removal of dye pollutants. Taking advantage of the combined benefits of graphene and magnetic nanoparticles, these MRGO nanocomposites exhibit excellent removal efficiency (over 91% for rhodamine B and over 94% for malachite green) and rapid separation from aqueous solution by an external magnetic field. Interestingly, the performance of the MRGO composites is strongly dependent on both the loading of Fe3O4 and the pH value. In addition, the adsorption behavior of this new adsorbent fits well with the Freundlich isotherm and the pseudo-second-order kinetic model. In further applications, real samples—including industrial waste water and lake water—have been treated using the MRGO composites. All the results demonstrate that the MRGO composites are effective adsorbents for removal of dye pollutants and thus could provide a new platform for dye decontamination.

Keywords: nanocomposites, graphene, Magnetic nanoparticles, removal, dye pollutants

References(60)

1

Hunger, K. Industrial Dyes: Chemistry, Properties, Applications; Wiley-VCH: Weinheim, Germany, 2003.
DOI
2

Christie, R. M. Environmental Aspects of Textile Dyeing; Woodhead Publishing: Great Abington, Cambridge, 2007.
DOI
3

Hai, F. I.; Yamamoto, K.; Fukushi, K. Hybrid treatment systems for dye wastewater. Crit. Rev. Environ. Sci. Technol. 2007, 37, 315–377.
DOI Google Scholar
4

Husain, Q. Potential applications of the oxidoreductive enzymes in the decolorization and detoxification of textile and other synthetic dyes from polluted water: A review. Crit. Rev. Biotechnol. 2006, 26, 201–221.
DOI Google Scholar
5

Horng, J. Y.; Huang, S. D. Phosphates, phosphites, and phosphides in environmental samples. Environ. Sci. Technol. 1993, 27, 1169–1174.
DOI Google Scholar
6

Kuo, W. G. Decolorizing dye wastewater with Fenton's reagent. Water Res. 1992, 26, 881–886.
DOI Google Scholar
7

Sujoy, K. D.; Jayati, B.; Akhil, R. D.; Arun, K. G. Adsorption behavior of rhodamine B on Rhizopus oryzae biomass. Langmuir 2006, 22, 7265–7272.
DOI Google Scholar
8

Legrini, O.; Oliveros, E.; Braun, A. M. Photochemical processes for water treatment. Chem. Rev. 1993, 93, 671–698.
DOI Google Scholar
9

Mohanty, K.; Naidu, J. T.; Meikap, B. C.; Biswas, M. N. Removal of crystal violet from wastewater by activated carbons prepared from rice husk. Ind. Eng. Chem. Res. 2006, 45, 5165–5171.
DOI Google Scholar
10

Chen, W.; Lu, W.; Yao, Y.; Xu, M. Highly efficient decomposition of organic dyes by aqueous-fiber phase transfer and in situ catalytic oxidation using fiber-supported cobalt phthalocyanine. Environ. Sci. Technol. 2007, 41, 6240–6245.
DOI Google Scholar
11

Pandit, P.; Basu, S. Removal of ionic dyes from water by solvent extraction using reverse micelles. Environ. Sci. Technol. 2004, 38, 2435–2442.
DOI Google Scholar
12

Yunus, R. F.; Zheng, Y. M.; K. Nanayakkara, G. N.; Chen, J. P. Electrochemical removal of rhodamine 6G by using RuO2 coated Ti DSA. Ind. Eng. Chem. Res. 2009, 48, 7466–7473.
DOI Google Scholar
13

Zhao, X. M.; Zhang, B. H.; Ai, K. L.; Zhang, G.; Cao, L. Y.; Liu, X. J.; Sun, H. M.; Wang, H. S.; Lu, L. H. Monitoring catalytic degradation of dye molecules on silver-coated ZnO nanowire arrays by surface-enhanced Raman spectroscopy. J. Mater. Chem. 2009, 19, 5547–5553.
DOI Google Scholar
14

Blackburn, R. S. Natural polysaccharides and their interactions with dye molecules: Applications in effluent treatment. Environ. Sci. Technol. 2004, 38, 4905–4909.
DOI Google Scholar
15

Sun, Z.; Li, C.; Wu, D. Removal of methylene blue from aqueous solution by adsorption onto zeolite synthesized from coal fly ash and its thermal regeneration. J. Chem. Technol. Biotechnol. 2010, 85, 845–850.
DOI Google Scholar
16

Asadullah, M.; Asaduzzaman, M.; Kabir, M. S.; Mostofa, M. G.; Miyazawa, T. Chemical and structural evaluation of activated carbon prepared from jute sticks for Brilliant Green dye removal from aqueous solution. J. Hazard. Mater. 2010, 174, 437–443.
DOI Google Scholar
17

Wang, P.; Shi, Q.; Shi, Y.; Clark, K. K.; Stucky, G. D.; Keller, A. A. Magnetic permanently confined micelle arrays for treating hydrophobic organic compound contamination. J. Am. Chem. Soc. 2009, 131, 182–188.
DOI Google Scholar
18

Sun, Z.; Wang, L.; Liu, P.; Wang, S.; Sun, B.; Jiang, D.; Xiao, F. Magnetically motive porous sphere composite and its excellent properties for the removal of pollutants in water by adsorption and desorption cycles. Adv. Mater. 2006, 18, 1968–1971.
DOI Google Scholar
19

Bekiari, V.; Lianos, P. Ureasil gels as a highly efficient sorbent for water purification. Chem. Mater. 2006, 18, 4142–4146.
DOI Google Scholar
20

Zhao, M.; Tang, Z.; Liu, P. Removal of methylene blue from aqueous solution with silica nano-sheets derived from vermiculite. J. Hazard. Mater. 2008, 158, 43–51.
DOI Google Scholar
21

Seredych, M.; Bandosz, T. J. Removal of cationic and ionic dyes on industrial-municipal sludge based composite adsorbents. Ind. Eng. Chem. Res. 2007, 46, 1786–1793.
DOI Google Scholar
22

Allen, M. J.; Tung, V. C.; Kaner, R. B. Honeycomb carbon: A review of graphene. Chem. Rev. 2010, 110, 132–145.
DOI Google Scholar
23

Cao, L. Y.; Liu, Y. L.; Zhang, B. H.; Lu, L. H. In situ controllable growth of Prussian blue nanocubes on reduced graphene oxide: Facile synthesis and their application as enhanced nanoelectrocatalyst for H2O2 reduction. ACS Appl. Mater. Interfaces 2010, 2, 2339–2346.
DOI Google Scholar
24

Ai, K. L.; Liu, Y. L.; Lu, L. H.; Cheng, X. L.; Huo, L. H. A novel strategy for making soluble graphene sheets cheaply by adopting an endogenous reducing agent. J. Mater. Chem., in press, DOI:10.1039/C0JM02865G.
Google Scholar
25

Su, Q.; Pang, S.; Alijani, V.; Li, C.; Feng, X.; Mullen, K. Composites of graphene with large aromatic molecules. Adv. Mater. 2009, 21, 3191–3195.
DOI Google Scholar
26

Loh, K.; Bao, Q.; Ang, P. K.; Yang, J. The chemistry of graphene. J. Mater. Chem. 2010, 20, 2277–2289.
DOI Google Scholar
27

Zacharia, R.; Ulbricht, H.; Hertel, T. Interlayer cohesive energy of graphite from thermal desorption of polyaromatic hydrocarbons. Phys. Rev. B 2004, 69, 155406.
DOI Google Scholar
28

Wu, Z.; Wang, D.; Ren, W.; Zhao, J.; Zhou, G.; Li, F.; Cheng, H. Anchoring hydrous RuO2 on graphene sheets for high-performance electrochemical capacitors. Adv. Funct. Mater. 2010, 20, 3595–3602.
DOI Google Scholar
29

Hu, J.; Zhong, L.; Song, W.; Wan, L. Synthesis of hierarchically structured metal oxides and their application in heavy metal ion removal. Adv. Mater. 2008, 20, 2977–2982.
DOI Google Scholar
30

Rocher, V.; Bee, A.; Siaugue, J. M.; Cabuil, V. Dye removal from aqueous solution by magnetic alginate beads crosslinked with epichlorohydrin. J. Hazard. Mater. 2010, 178, 434–439.
DOI Google Scholar
31

Zhai, Y. M.; Zhai, J. F.; Zhou, M.; Dong, S. J. Ordered magnetic core–manganese oxide shell nanostructures and their application in water treatment. J. Mater. Chem. 2009, 19, 7030–7035.
DOI Google Scholar
32

Cong, H. P.; He, J. J.; Lu, Y.; Yu, S. H. Water-soluble magnetic-functionalized reduced graphene oxide sheets: In situ synthesis and magnetic resonance imaging applications. Small 2009, 6, 169–173.
DOI Google Scholar
33

Chandra, V.; Park, J.; Chun, Y.; Lee, J. W.; Hwang, I.; Kim, K. S. Water-dispersible magnetite–reduced graphene oxide composites for arsenic removal. ACS Nano 2010, 4, 3979–3986.
DOI Google Scholar
34

Zhang, M.; Lei, D.; Yin, X.; Chen, L.; Li, Q.; Wang, Y.; Wang, T. Magnetite/graphene composites: Microwave irradiation synthesis and enhanced cycling and rate performances for lithium ion batteries. J. Mater. Chem. 2010, 20, 5538–5543.
DOI Google Scholar
35

Shen, J.; Hu, Y.; Shi, M.; Li, N.; Ma, H.; Ye, M. One step synthesis of graphene oxide–magnetic nanoparticle composite. J. Phys. Chem. C 2010, 114, 1498–1503.
DOI Google Scholar
36

Liang, J.; Xu, Y.; Sui, D.; Zhang, L.; Huang, Y.; Ma, Y.; Li, F.; Chen, Y. Flexible, magnetic, and electrically conductive graphene/Fe3O4 paper and its application for magnetic-controlled switches. J. Phys. Chem. C 2010, 114, 17465–17471.
DOI Google Scholar
37

Wang, H.; Robinson, J. T.; Li, X.; Dai, H. Solvothermal reduction of chemically exfoliated graphene sheets. J. Am. Chem. Soc. 2009, 131, 9910–9911.
DOI Google Scholar
38

Dubin, S.; Gilje, S.; Wang, K.; Tung, V. C.; Cha, K.; Hall, A. S.; Farrar, J.; Varshneya, R.; Yang, Y.; Kaner, R. B. A one-step, solvothermal reduction method for producing reduced graphene oxide dispersions in organic solvents. ACS Nano, 2010, 4, 3845–3852.
DOI Google Scholar
39

Deng, H.; Li, X.; Peng, Q.; Wang, X.; Chen, J.; Li, Y. Monodisperse magnetic single-crystal ferrite microspheres. Angew. Chem., Int. Ed. 2005, 44, 2782–2785.
DOI Google Scholar
40

Yang, X. Y.; Zhang, X. Y.; Ma, Y. F.; Huang, Y.; Wang, Y. S.; Chen, Y. S. Superparamagnetic graphene oxide–Fe3O4 nanoparticles hybrid for controlled targeted drug carriers. J. Mater. Chem. 2009, 19, 2710–2714.
DOI Google Scholar
41

Xuan, S.; Wang, Y. J.; Yu, J. C.; Leung, K. C. Tuning the grain size and particle size of superparamagnetic Fe3O4 microparticles. Chem. Mater. 2009, 21, 5079–5087.
DOI Google Scholar
42

Zhu, C.; Guo, S.; Fang, Y.; Dong, S. Reducing sugar: New functional molecules for the green synthesis of graphene nanosheets. ACS Nano 2010, 4, 2429–2437.
DOI Google Scholar
43

Lu, L. H.; Randjelovic, I.; Capek, R.; Gaponik, N.; Yang, J. H.; Zhang, H. J.; Eychmuller, A. Controlled fabrication of gold-coated 3D ordered colloidal crystal films and their application in surface-enhanced Raman spectroscopy. Chem. Mater. 2005, 17, 5731–5736.
DOI Google Scholar
44

Lu, L. H.; Ai, K. L.; Ozaki, Y. Environmentally friendly synthesis of highly monodisperse biocompatible gold nanoparticles with urchin-like shape. Langmuir 2008, 24, 1058–1063.
DOI Google Scholar
45

Warren, B. E. X-ray Diffraction; Addison-Wesley: London, 1969.
46

Guo, H. L.; Wang, X. F.; Qian, Q. Y.; Wang, F. B.; Xia, X. H. A green approach to the synthesis of graphene nanosheets. ACS Nano 2009, 3, 2653–2659.
DOI Google Scholar
47

Ge, J.; Hu, Y.; Biasini, M.; Beyermann, W. P.; Yin, Y. Superparamagnetic magnetite colloidal nanocrystal clusters. Angew. Chem., Int. Ed. 2007, 46, 4342–4345.
DOI Google Scholar
48

McAllister, M. J.; Li, J. L.; Adamson, D. H.; Schniepp, H. C.; Abdala, A. A.; Liu, J.; Herrera-Alonso, M.; Milius, D. L.; Car, R.; Prud'homme, R. K.; Aksay, I. A. Single sheet functionalized graphene by oxidation and thermal expansion of graphite. Chem. Mater. 2007, 19, 4396–4404.
DOI Google Scholar
49

Yang, H. F.; Li, F. H.; Shan, C. S.; Han, D. X.; Zhang, Q. X.; Niu, L.; Ivaska, A. Covalent functionalization of chemically converted graphene sheets via silane and its reinforcement. J. Mater. Chem. 2009, 19, 4632–4638.
DOI Google Scholar
50

Park, S.; An, J.; Jung, I.; Piner, R. D.; An, S. J.; Li, X.; Velamakanni, A.; Ruoff, R. S. Colloidal suspensions of highly reduced graphene oxide in a wide variety of organic solvents. Nano Lett. 2009, 9, 1593–1597.
DOI Google Scholar
51

Zhang, L.; Qiao, S. Z.; Jin, Y. G.; Chen, Z. G.; Gu, H. C.; Lu, G. Q. Magnetic hollow spheres of periodic mesoporous organosilica and Fe3O4 nanocrystals: Fabrication and structure control. Adv. Mater. 2008, 20, 805–809.
DOI Google Scholar
52

Liu, Y. L.; Ai, K. L.; Cheng, X. L.; Huo, L. H.; Lu, L. H. Gold-nanocluster-based fluorescent sensors for highly sensitive and selective detection of cyanide in water. Adv. Funct. Mater. 2010, 20, 951–956.
DOI Google Scholar
53

Hameed, B. H.; El-Khaiary, M. I. Batch removal of malachite green from aqueous solutions by adsorption on oil palm trunk fibre: Equilibrium isotherms and kinetic studies. J. Hazard. Mater. 2008, 154, 237–244.
DOI Google Scholar
54

Ngah, W. S. W.; Ariff, N. F. M.; Hashim, A.; Hanaf, M. A. K. M. Malachite green adsorption onto chitosan coated bentonite beads: Isotherms, kinetics and mechanism. Clean—Soil, Air, Water 2010, 38, 394–400.
DOI Google Scholar
55

Vijayakumar, G.; Yoo, C. K.; Elango, K. G. P.; Dharmendirakumar, M. Adsorption characteristics of rhodamine B from aqueous solution onto baryte. Clean—Soil, Air, Water 2010, 38, 202–209.
DOI Google Scholar
56

Langmuir, I. The adsorption of gases on plane surfaces of glass, mica and platinum. J. Am. Chem. Soc. 1918, 40, 1361–1403.
DOI Google Scholar
57

Freundlich, H. M. F. Über die adsorption in Lösungen. Z. Phys. Chem. 1906, 57A, 385–470.
DOI Google Scholar
58

Ai, K. L.; Liu, Y. L.; Lu, L. H. Hydrogen-bonding recognition-induced color change of gold nanoparticles for visual detection of melamine in raw milk and infant formula. J. Am. Chem. Soc. 2009, 131, 9496–9497.
DOI Google Scholar
59

Zhang, B. H.; Wang, H. S.; Lu, L. H.; Ai, K. L.; Zhang, G.; Cheng, X. L. Large-area silver-coated silicon nanowire arrays for molecular sensing using surface-enhanced Raman spectroscopy. Adv. Funct. Mater. 2008, 18, 2348–2355.
DOI Google Scholar
60

Hummers, W. S.; Offeman, R. E. Preparation of graphitic oxide. J. Am. Chem. Soc. 1958, 80, 1339–1339.
DOI Google Scholar
File
nr-4-6-550_ESM.pdf (2.3 MB)
Publication history
Copyright
Acknowledgements

Publication history

Received: 22 November 2010
Revised: 16 December 2010
Accepted: 18 January 2011
Published: 18 February 2011
Issue date: June 2011

Copyright

© Tsinghua University Press and Springer‐Verlag Berlin Heidelberg 2011

Acknowledgements

Acknowledgements

Financial support by the National Basic Research Program of China (973 Program; No.2010CB933600), and the "Hundred Talents Project" of the Chinese Academy of Sciences is gratefully acknowledged.

Return