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Analytical and Bioanalytical Chemistry

, Volume 409, Issue 10, pp 2665–2674 | Cite as

Graphene oxide/Fe3O4 as sorbent for magnetic solid-phase extraction coupled with liquid chromatography to determine 2,4,6-trinitrotoluene in water samples

  • Luciana Costa dos Reis
  • Lorena VidalEmail author
  • Antonio CanalsEmail author
Research Paper

Abstract

A fast, simple, economical, and environmentally friendly magnetic solid-phase extraction (MSPE) procedure has been developed to preconcentrate 2,4,6-trinitrotoluene (TNT) from water samples prior to determination by liquid chromatography-UV-Vis employing graphene oxide/Fe3O4 nanocomposite as sorbent. The nanocomposite synthesis was investigated, and the MSPE was optimized by a multivariate approach. The optimum MSPE conditions were 40 mg of nanocomposite, 10 min of vortex extraction, 1 mL of acetonitrile as eluent, and 6 min of desorption in an ultrasonic bath. Under the optimized experimental conditions, the method was evaluated to obtain a preconcentration factor of 153. The linearity of the method was studied from 1 to 100 μg L−1 (N = 5), obtaining a correlation coefficient of 0.994. The relative standard deviation and limit of detection were found to be 12% (n = 6, 10 μg L−1) and 0.3 μg L−1, respectively. The applicability of the method was investigated, analyzing three types of water samples (i.e., reservoir and drinking water and effluent wastewater) and recovery values ranged between 87 and 120% (50 μg L−1 spiking level), showing that the matrix had a negligible effect upon extraction. Finally, the semiquantitative Eco-Scale metrics confirmed the greenness of the developed method.

Keywords

Graphene oxide/Fe3O4 nanocomposite Liquid chromatography-UV-Vis Magnetic solid-phase extraction 2,4,6-Trinitrotoluene Water samples 

Notes

Acknowledgements

The authors would like to thank the Ministry of Science and Innovation of Spain (project no. CTQ2011-23968) for the financial support and L. Costa thanks the Capes Foundation within the Ministry of Education in Brazil (Process 12013/13-7).

Compliance with ethical standards

Conflict of interest

The authors declare that they have no conflicts of interest.

Supplementary material

216_2017_211_MOESM1_ESM.pdf (261 kb)
ESM 1 (PDF 260 kb)

References

  1. 1.
    Stoller MD, Park S, Zhu Y, An J, Ruoff RS. Graphene-based ultracapacitors. Nano Lett. 2008;8:3498–502.CrossRefGoogle Scholar
  2. 2.
    Lee C, Wei X, Kysar JW, Hone J. Measurement of the elastic properties and intrinsic strength of monolayer graphene. Science. 2008;321:385–88.CrossRefGoogle Scholar
  3. 3.
    Bolotin KI, Sikes KJ, Jiang Z, Klima M, Fudenberg G, Hone J, et al. Ultrahigh electron mobility in suspended graphene. Solid State Commun. 2008;146:351–55.CrossRefGoogle Scholar
  4. 4.
    Liu Q, Shi J, Zeng L, Wang T, Cai Y, Jiang G. Evaluation of graphene as an advantageous adsorbent for solid-phase extraction with chlorophenols as model analytes. J Chromatogr A. 2011;1218:197–204.CrossRefGoogle Scholar
  5. 5.
    Chen J, Zou J, Zeng J, Song X, Ji J, Wang Y, et al. Preparation and evaluation of graphene-coated solid-phase microextraction fiber. Anal Chim Acta. 2010;678:44–9.CrossRefGoogle Scholar
  6. 6.
    Zhang H, Lee HK. Plunger-in-needle solid-phase microextraction with graphene-based sol–gel coating as sorbent for determination of polybrominated diphenyl ethers. J Chromatogr A. 2011;1218:4509–16.CrossRefGoogle Scholar
  7. 7.
    Zhang S, Du Z, Li G. Layer-by-layer fabrication of chemical-bonded graphene coating for solid-phase microextraction. Anal Chem. 2011;83:7531–41.CrossRefGoogle Scholar
  8. 8.
    Ponnusamy VK, Jen JF. A novel graphene nanosheets coated stainless steel fiber for microwave assisted headspace solid phase microextraction of organochlorine pesticides in aqueous samples followed by gas chromatography with electron capture detection. J Chromatogr A. 2011;1218:6861–68.CrossRefGoogle Scholar
  9. 9.
    Hummers WS, Offeman RE. Preparation of graphitic oxide. J Am Chem Soc. 1958;80:1339–39.CrossRefGoogle Scholar
  10. 10.
    Fritz JS. Analytical solid-phase extraction. New York: Wiley; 1999.Google Scholar
  11. 11.
    Han Q, Wang Z, Xia J, Xia L, Chen S, Zhang XQ, et al. Graphene as an efficient sorbent for the SPE of organochlorine pesticides in water samples coupled with GC-MS. J Sep Sci. 2013;36:3586–91.CrossRefGoogle Scholar
  12. 12.
    Wang Z, Han Q, Xia J, Xia L, Ding M, Tang J. Graphene-based solid-phase extraction disk for fast separation and preconcentration of trace polycyclic aromatic hydrocarbons from environmental water samples. J Sep Sci. 2013;36:1834–42.CrossRefGoogle Scholar
  13. 13.
    Wu J, Chen L, Mao P, Lu Y, Wang HZ. Determination of chloramphenicol in aquatic products by graphene-based SPE coupled with HPLC-MS/MS. J Sep Sci. 2012;35:3586–92.CrossRefGoogle Scholar
  14. 14.
    Luo X, Zhang FF, Ji S, Yang B, Liang X. Graphene nanoplatelets as a highly efficient solid-phase extraction sorbent for determination of phthalate esters in aqueous solution. Talanta. 2014;120:71–5.CrossRefGoogle Scholar
  15. 15.
    Wang SL, Hu S, Xu H. Analysis of aldehydes in human exhaled breath condensates by in-tube SPME-HPLC. Anal Chim Acta. 2015;900:67–75.CrossRefGoogle Scholar
  16. 16.
    Pawliszyn J. Solid Phase Microextraction. Theory and Practice. New York: Wiley; 1997.Google Scholar
  17. 17.
    He H, Klinowski J, Forster M, Lerf A. A new structural model for graphite oxide. Chem Phys Lett. 1998;287:53–6.CrossRefGoogle Scholar
  18. 18.
    Sitko R, Zawisza B, Malicka E. Graphene as a new sorbent in analytical chemistry. Trends Anal Chem. 2013;51:33–43.CrossRefGoogle Scholar
  19. 19.
    Yang X, Li J, Wen T, Ren X, Huang Y, Wang X. Adsorption of naphthalene and its derivatives on magnetic graphene composites and the mechanism investigation. Colloid Surface A. 2013;422:118–25.CrossRefGoogle Scholar
  20. 20.
    Sitko R, Turek E, Zawisza B, Malicka E, Talik E, Heimann J, et al. Adsorption of divalent metal ions from aqueous solutions using graphene oxide. Dalton Trans. 2013;42:5682–89.CrossRefGoogle Scholar
  21. 21.
    Liu Q, Shi J, Sun J, Wang T, Zeng L, Jiang G. Graphene and graphene oxide sheets supported on silica as versatile and high-performance adsorbents for solid-phase extraction. Angew Chem Int Ed. 2011;50:5913–17.CrossRefGoogle Scholar
  22. 22.
    Xu L, Feng J, Li J, Liu X, Jiang S. Graphene oxide bonded fused-silica fiber for solid-phase microextraction-gas chromatography of polycyclic aromatic hydrocarbons in water. J Sep Sci. 2012;35:93–100.CrossRefGoogle Scholar
  23. 23.
    Meng J, Shi C, Wei B, Yu W, Deng C, Zhang X. Preparation of Fe3O4@C@PANI magnetic microspheres for the extraction and analysis of phenolic compounds in water samples by gas chromatography-mass spectrometry. J Chromatogr A. 2011;1218:2841–47.CrossRefGoogle Scholar
  24. 24.
    Sasaki T, Tanaka S. Adsorption behavior of some aromatic compounds on hydrophobic magnetite for magnetic separation. J Hazard Mater. 2011;196:327–34.CrossRefGoogle Scholar
  25. 25.
    Zhang X, Niu H, Pan Y, Shi Y, Cai Y. Modifying the surface of Fe3O4/SiO2 magnetic nanoparticles with C18/NH2 mixed group to get an efficient sorbent for anionic organic pollutants. J Colloid Interface Sci. 2011;362:107–12.CrossRefGoogle Scholar
  26. 26.
    Tang H, Zhu L, Yu C, Shen X. Selective photocatalysis mediated by magnetic molecularly imprinted polymers. Sep Purif Technol. 2012;95:165–71.CrossRefGoogle Scholar
  27. 27.
    Li S, Gong Y, Yang Y, He C, Hu L, Zhu L, et al. Recyclable CNTs/Fe3O4 magnetic nanocomposites as adsorbents to remove bisphenol A from water and their regeneration. Chem Eng J. 2015;260:231–39.CrossRefGoogle Scholar
  28. 28.
    Sun T, Yang J, Li L, Wang X, Li X, Jin Y. Preparation of graphene sheets with covalently bonded Fe3O4 for magnetic solid-phase extraction applied to organochlorine pesticides in orange juice. Chromatographia. 2016;79:345–53.CrossRefGoogle Scholar
  29. 29.
    Han Q, Wang Z, Xia J, Chen S, Zhang X, Ding M. Facile and tunable fabrication of Fe3O4/graphene oxide nanocomposites and their application in the magnetic solid-phase extraction of polycyclic aromatic hydrocarbons from environmental water samples. Talanta. 2012;101:388–95.CrossRefGoogle Scholar
  30. 30.
    Aguilar-Arteaga K, Rodriguez JA, Miranda JM, Medina J, Barrado E. Determination of non-steroidal anti-inflammatory drugs in wastewaters by magnetic matrix solid phase dispersion–HPLC. Talanta. 2010;80:1152–57.CrossRefGoogle Scholar
  31. 31.
    Šafařı́k I, Šafařı́ková M. Detection of low concentrations of malachite green and crystal violet in water. Water Res. 2002;36:196-200Google Scholar
  32. 32.
    Taghvimi A, Hamishehkar H, Ebrahimi M. Magnetic nano graphene oxide as solid phase extraction adsorbent coupled with liquid chromatography to determine pseudoephedrine in urine samples. J Chromatogr B. 2016;1009-1010:66–72.CrossRefGoogle Scholar
  33. 33.
    Zeng S, Gan N, Weideman-Mera R, Cao Y, Li T, Sang W. Enrichment of polychlorinated biphenyl 28 from aqueous solutions using Fe3O4 grafted graphene oxide. Chem Eng J. 2013;218:108–15.CrossRefGoogle Scholar
  34. 34.
    Stucki H. Toxicity and degradation of explosives. Chimia. 2004;58:409–13.CrossRefGoogle Scholar
  35. 35.
    Keith L, Telliard W. Priority pollutants I—a perspective view. Environ Sci Technol. 1979;13:416–23.CrossRefGoogle Scholar
  36. 36.
    Talmage SS, Opresko DM, Maxwell CJ, Welsh CJE, Cretella FM, Reno PH, et al. Reviews of Environmental Contamination and Toxicology. New York: Springer; 1999.Google Scholar
  37. 37.
    Psillakis E, Kalogerakis N. Solid-phase microextraction versus single-drop microextraction for the analysis of nitroaromatic explosives in water samples. J Chromatogr A. 2011;938:113–20.CrossRefGoogle Scholar
  38. 38.
    Psillakis E, Kalogerakis N. Application of solvent microextraction to the analysis of nitroaromatic explosives in water samples. J Chromatogr A. 2001;907:211–19.CrossRefGoogle Scholar
  39. 39.
    Psillakis E, Mantzavinos D, Kalogerakis N. Development of a hollow fibre liquid phase microextraction method to monitor the sonochemical degradation of explosives in water. Anal Chim Acta. 2004;501:3–10.CrossRefGoogle Scholar
  40. 40.
    Cortada C, Vidal L, Canals A. Determination of nitroaromatic explosives in water samples by direct ultrasound-assisted dispersive liquid–liquid microextraction followed by gas chromatography–mass spectrometry. Talanta. 2011;85:2546–52.CrossRefGoogle Scholar
  41. 41.
    Wei Y, Han B, Hu X, Lin Y, Wang X, Deng X. Synthesis of Fe3O4 nanoparticles and their magnetic properties. Procedia Eng. 2012;27:632–7.CrossRefGoogle Scholar
  42. 42.
    Shih CJ, Lin S, Sharma R, Strano MS, Blankschtein D. Understanding the pH-dependent behavior of graphene oxide aqueous solutions: a comparative experimental and molecular dynamics simulation study. J Am Chem Soc. 2012;28:235–41.Google Scholar
  43. 43.
    Thermo Scientific database (November, 2016), www.lasurface.com
  44. 44.
    Draper NR. Plackett and Burman designs. In: Kotz S, Johnson L, editors. Encyclopedia of Statistical Sciences. New York: John Wiley & Sons; 1985. p. 754–8.Google Scholar
  45. 45.
    Gałuszka A, Konieczka P, Migaszewski ZM, Namiesnik J. Analytical Eco-Scale for assessing the greenness of analytical procedures. Trends Anal Chem. 2012;37:61–72.CrossRefGoogle Scholar

Copyright information

© Springer-Verlag Berlin Heidelberg 2017

Authors and Affiliations

  1. 1.Departamento de Química Analítica, Nutrición y Bromatología e Instituto Universitario de MaterialesUniversidad de AlicanteAlicanteSpain

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